Thematische Bibliographien / Overall alkaline water splitting

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Auswahl der wissenschaftlichen Literatur zum Thema „Overall alkaline water splitting“

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Veröffentlicht am 25. Mai 2024

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Zeitschriftenartikel zum Thema "Overall alkaline water splitting"

Liu, Yang, Fengmei Wang, Tofik Ahmed Shifa, Jie Li, Jing Tai, Yu Zhang, Junwei Chu, Xueying Zhan, Chongxin Shan und Jun He. „Hierarchically heterostructured metal hydr(oxy)oxides for efficient overall water splitting“. Nanoscale 11, Nr. 24 (2019): 11736–43. http://dx.doi.org/10.1039/c9nr02988e.

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Liang, Shuqin, Meizan Jing, Tiju Thomas, Jian Liu, Haichuan Guo, J. Paul Attfield, Ali Saad, Hangjia Shen und Minghui Yang. „FeNi3–FeNi3N – a high-performance catalyst for overall water splitting“. Sustainable Energy & Fuels 4, Nr. 12 (2020): 6245–50. http://dx.doi.org/10.1039/d0se01491e.

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Liu, Bingrui, Ning Zhang und Mingming Ma. „Cobalt-based nanosheet arrays as efficient electrocatalysts for overall water splitting“. Journal of Materials Chemistry A 5, Nr. 33 (2017): 17640–46. http://dx.doi.org/10.1039/c7ta04248e.

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Amin, Bahareh Golrokh, Abdurazag T. Swesi, Jahangir Masud und Manashi Nath. „CoNi2Se4 as an efficient bifunctional electrocatalyst for overall water splitting“. Chemical Communications 53, Nr. 39 (2017): 5412–15. http://dx.doi.org/10.1039/c7cc01489a.

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Electrodeposited CoNi₂Se₄ shows excellent electrocatalytic activity for OER and HER in alkaline medium with a low overpotential at 10 mA cm⁻² (160 mV for OER, and 210 mV for HER).

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Duan, Wei, Shixing Han, Zhonghai Fang, Zhaohui Xiao und Shiwei Lin. „In Situ Filling of the Oxygen Vacancies with Dual Heteroatoms in Co3O4 for Efficient Overall Water Splitting“. Molecules 28, Nr. 10 (16.05.2023): 4134. http://dx.doi.org/10.3390/molecules28104134.

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Electrocatalytic water splitting is a crucial area in sustainable energy development, and the development of highly efficient bifunctional catalysts that exhibit activity toward both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is of paramount importance. Co3O4 is a promising candidate catalyst, owing to the variable valence of Co, which can be exploited to enhance the bifunctional catalytic activity of HER and OER through rational adjustments of the electronic structure of Co atoms. In this study, we employed a plasma-etching strategy in combination with an in situ filling of heteroatoms to etch the surface of Co3O4, creating abundant oxygen vacancies, while simultaneously filling them with nitrogen and sulfur heteroatoms. The resulting N/S-VO-Co3O4 exhibited favorable bifunctional activity for alkaline electrocatalytic water splitting, with significantly enhanced HER and OER catalytic activity compared to pristine Co3O4. In an alkaline overall water-splitting simulated electrolytic cell, N/S-VO-Co3O4 || N/S-VO-Co3O4 showed excellent overall water splitting catalytic activity, comparable to noble metal benchmark catalysts Pt/C || IrO2, and demonstrated superior long-term catalytic stability. Additionally, the combination of in situ Raman spectroscopy with other ex situ characterizations provided further insight into the reasons behind the enhanced catalyst performance achieved through the in situ incorporation of N and S heteroatoms. This study presents a facile strategy for fabricating highly efficient cobalt-based spinel electrocatalysts incorporated with double heteroatoms for alkaline electrocatalytic monolithic water splitting.

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Li, Ying, Fumin Li, Yue Zhao, Shu-Ni Li, Jing-Hui Zeng, Hong-Chang Yao und Yu Chen. „Iron doped cobalt phosphide ultrathin nanosheets on nickel foam for overall water splitting“. Journal of Materials Chemistry A 7, Nr. 36 (2019): 20658–66. http://dx.doi.org/10.1039/c9ta07289f.

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Sun, Jianrui, Saisai Li, Qiaoqiao Zhang und Jingqi Guan. „Iron–cobalt–nickel trimetal phosphides as high-performance electrocatalysts for overall water splitting“. Sustainable Energy & Fuels 4, Nr. 9 (2020): 4531–37. http://dx.doi.org/10.1039/d0se00694g.

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Liu, Xin, Jinmei Dong, Bo You und Yujie Sun. „Competent overall water-splitting electrocatalysts derived from ZIF-67 grown on carbon cloth“. RSC Advances 6, Nr. 77 (2016): 73336–42. http://dx.doi.org/10.1039/c6ra17030g.

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Vigil, Julian A., und Timothy N. Lambert. „Nanostructured cobalt phosphide-based films as bifunctional electrocatalysts for overall water splitting“. RSC Advances 5, Nr. 128 (2015): 105814–19. http://dx.doi.org/10.1039/c5ra24562a.

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Nanostructured cobalt phosphide-based films (Co-PP) were shown to be effective bifunctional electrocatalysts for the hydrogen and oxygen evolution reactions. A symmetrical alkaline electrolysis cell demonstrated low overpotential for water splitting.

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Wei, Yi, Cheol-Hwan Shin, Caleb Gyan-Barimah, Emmanuel Batsa Tetteh, Gisang Park und Jong-Sung Yu. „Positive self-reconstruction in an FeNiMo phosphide electrocatalyst for enhanced overall water splitting“. Sustainable Energy & Fuels 5, Nr. 22 (2021): 5789–97. http://dx.doi.org/10.1039/d1se01541a.

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Binder-free FeNiMoP synthesized by a simple two-step method shows interesting structural self-reconstruction and demonstrates remarkably high electrocatalytic overall water splitting performance in alkaline conditions.

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Dissertationen zum Thema "Overall alkaline water splitting"

Jiang, Tao. „Development of Alkaline Electrolyzer Electrodes and Their Characterization in Overall Water Splitting“. Thesis, Bourgogne Franche-Comté, 2020. http://www.theses.fr/2020UBFCA006.

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La décomposition électrolytique de l’eau en hydrogène et oxygène à l’aide d’électricité renouvelable générée par les courants marins ou à partir d’énergie éolienne ou solaire, constitue l’une des voies les plus propres et directes pour produire de l’hydrogène. Toutefois, la production de grands volumes d’hydrogène par décomposition électrolytique de l’eau comporte un verrou technologique qui réside dans la forte surtension à vaincre à l’anode où de l’oxygène est dégagé. Ce travail de thèse s’est attaché donc à mettre au point des matériaux d’électrodes capables de catalyser de l’eau en oxygène de façon efficace et stable, en utilisant des éléments chimiques suffisamment abondants sur terre. Pour cela nous avons exploré des composés présentant des porosités à structures hiérarchiques et des procédés de préparation efficaces, aisées à mettre en œuvre et susceptibles d’un usage à l’échelle industrielle. Nous avons développé deux types d’électrocatalyseurs d’oxydation de l’eau en oxygène en mettant au point deux voies de préparation impliquant chacune une phase d’activation in situ. Le premier type est une mousse de nickel dopée à la fois avec des cristaux de nickel, des nanoparticules de tétroxyde de tricobalt et des nanofeuilles d’oxyde de graphène via nickelage électrolytique, suivi d’une activation électrochimique in situ pour former de l’hydroxyde de nickel et des nano-plaques d’oxy-hydroxyde du même métal. Ce catalyseur hybride s’est avéré avoir des performances électrocatalytiques de bon niveau, comparables à celles des électrodes à base de métaux nobles qui sont disponibles dans l’état actuel de la technique ; il a en outre fait preuve d’une excellente stabilité en fonctionnement. Ces propriétés remarquables semblent liées à la fois aux dépôts formés sur la mousse de nickel par les différentes phases actives citées, aux nanoparticules d’oxy-hydroxyde de nickel, ainsi qu’aux effets de synergie qu’elles y induisent. Le second type d’électrocatalyseurs a été obtenu en combinant la projection thermique (HVOF) et un processus d’activation chimique puis électrochimique. Le matériau résultant possède de nanocouches du type jamborite formée in situ, sur la matrice poreuse à structure hiérarchique. Le catalyseur développé dans ce travail présente non seulement une surtension et une pente de Tafel exceptionnellement faibles, mais également une stabilité remarquable. Ces performances sont dues à un puissant effet de synergie dans laquelle interviennent la grande activité intrinsèque des nanofeuilles de jamborite et la grande rapidité des transports d’électrons et d’ions assurée par l'architecture poreuse hiérarchique. Il convient de noter que cette nouvelle méthodologie a le potentiel de produire des électrodes de grandes tailles apte à l’électrolyse alcaline de l'eau et crée ainsi de nouvelles perspectives dans le cadre de la conception d'électrocatalyseurs à la fois très actifs et stables. Nous avons également développé, initialement, des électrocatalyseurs destinés à la réduction de l’eau en hydrogène, qui impliquent également une activation électrochimique in situ. Ces électrodes peuvent être ainsi couplées aux électrodes précitées d’oxydation de l’eau en oxygène pour former des cellules électrochimiques complètes à deux électrodes, dont les performances rivalisent avec celles développées par le couple dioxyde de ruthénium/platine qui représente le meilleur état de la technique dans le cadre de la production d’hydrogène et d’oxygène par électrolyse de l’eau. En résumé, en combinant des techniques conventionnelles de revêtement et d’activation électrochimique in situ, ce travail a permis de développer une méthodologie de préparation d'électrodes catalytiques offrant de hautes performances et susceptibles de commercialisation. La technique d’activation électrochimique in situ exploite un comportement d'auto-optimisation dynamique qui est aisé à mettre en œuvre, facilement adaptable, efficace et respectueux de l'environnement
Splitting water into hydrogen and oxygen by electrolysis using electricity from intermittent ocean current, wind, or solar energies is one of the easiest and cleanest routes for high-purity hydrogen production and an effective way to store the excess electrical power without leaving any carbon footprints. The key dilemma for efficient large-scale production of hydrogen by splitting of water via the hydrogen and oxygen evolution reactions is the high overpotential required, especially for the oxygen evolution reaction. Hence, engineering highly active and stable earth-abundant oxygen evolution electrocatalysts with three-dimensional hierarchical porous architecture via facile, effective and commercial means is the main objective of the present PhD study. Finally, we developed two kinds of good performance oxygen evolution electrocatalysts through two different way combined with in situ electrochemical activation.For the first oxygen evolution electrocatalyst, we report a codoped nickel foam by nickel crystals, tricobalt tetroxide nanoparticles, graphene oxide nanosheets, and in situ generated nickel hydroxide and nickel oxyhydroxide nanoflakes via facile electrolytic codeposition in combination with in situ electrochemical activation as a promising electrocatalyst for oxygen evolution reaction. Notably, this hybrid catalyst shows good electrocatalytic performance, which is comparable to the state-of-the-art noble catalysts. The hybrid catalyst as an electrocatalytically-active and robust oxygen evolution electrocatalyst also exhibits strong long-term electrochemical durability. Such a remarkable performance can be benefiting from the introduced active materials deposited on nickel foam, in situ generated nickel oxyhydroxide nanoflakes and their synergistic effects. It could potentially be implemented in large-scale water electrolysis systems.For the second oxygen evolution electrocatalyst, a facile and efficient means of combining high-velocity oxy-fuel spraying followed by chemical activation, and in situ electrochemical activation based on oxygen evolution reaction has been developed to obtain a promising self-supported oxygen evolution electrocatalyst with lattice-distorted Jamborite nanosheets in situ generated on the three-dimensional hierarchical porous framework. The catalyst developed in this work exhibits not only exceptionally low overpotential and Tafel slope, but also remarkable stability. Such a remarkable feature of this catalyst lies in the synergistic effect of the high intrinsic activity arising from the lattice-dislocated Jamborite nanosheets as the highly active substance, and the accelerated electron/ion transport associated with the hierarchical porous architecture. Notably, this novel methodology has the potential to produce large-size-electrode for alkaline water electrolyzer, which can provide new dimensions in design of highly active and stable self-supported electrocatalysts.Furthermore, we have also initially developed good hydrogen evolution electrocatalysts upon in situ electrochemical activation, coupled with the obtained superior oxygen evolution electrocatalysts forming two-electrode configurations, respectively, both of which rivalled the integrated state-of-the-art ruthenium dioxide-platinum electrode in alkaline overall water splitting.In summary, a methodology of fabricating easy-to-commercial, high performance catalytic electrodes by combining general coating processes with in situ electrochemical activation has been realized and well developed. The in situ electrochemical activation mentioned above is a dynamic self-optimization behavior which is facile, flexible, effective and eco-friendly, as a strategy of fabricating self-supported electrodes for efficient and durable overall water splitting. We hope our work can promote advanced development toward large-scale hydrogen production using excess electrical power whenever and wherever available

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Sommers, Jacob. „Towards Photocatalytic Overall Water Splitting via Small Organic Shuttles“. Thesis, Université d'Ottawa / University of Ottawa, 2016. http://hdl.handle.net/10393/34607.

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This thesis studies the development of a new method for photochemical overall water splitting using a small organic shuttle. In Section 2, BiVO4, was studied to determine the CO2 reduction mechanism and how catalytic activity decays. BiVO4 catalysts were capable of producing a maximum of 200 μmol of methanol per gram of catalyst from CO2 in basic media, and later decomposed by BiVO4. The decay of BiVO4¬ was studied by x-ray diffraction and scanning electron microscopy, demonstrating reversible decomposition of BiVO4. BiVO4 is etched, leeching vanadium into solution, while nanoparticles of bismuth oxide are deposited on the surface of BiVO4. In Section 3, ferrocyanide salts, an aqueous, cheap, and abundant photocatalyst was used for the first time to dehydrogenate aqueous formaldehyde selectively into formate and hydrogen. The catalyst is capable of record turnovers and turnover frequencies for formaldehyde dehydrogenation catalysts. A preliminary mechanism was proposed from experimental and computational data.

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Song, Yang. „Design of metal silicide nanoparticles in molten salts : electrocatalytic and magnetic properties“. Electronic Thesis or Diss., Sorbonne université, 2021. https://accesdistant.sorbonne-universite.fr/login?url=https://theses-intra.sorbonne-universite.fr/2021SORUS498.pdf.

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Les siliciures de métaux de transition sont une famille de composés intermétalliques, qui ont été largement étudiés en tant que matériaux fonctionnels dans les circuits intégrés, la thermoélectricité, la supraconductivité, le magnétisme et la catalyse hétérogène. La nanostructuration offre la possibilité repousser les frontières de la science de ces matériaux avec de nouvelles phases et des propriétés diverses. Cependant, l'énergie de liaison relativement élevée des siliciures de métaux de transition nécessite généralement une température élevée pour leur formation, ce qui n'est pas propice à la conception de nanomatériaux et n'est pas compatible avec les méthodes de synthèse colloïdales traditionnelles. Dans cette thèse, des synthèses en sels fondus basées sur l'insertion d'éléments dans des nanoparticules sont développées. Des nanoparticules de siliciure de métal de transition (M-Si, M=Ni, Fe, NiFe, Co) et un silicophosphure de nickel ternaire sont cristallisés dans des solvants inorganiques à haute température, où un environnement dilué et sans carbone est fourni. Les nanoparticules de siliciures obtenues sont étudiées en électrocatalyse de l'oxydation de l'eau alcaline et du magnétisme. Les siliciures de NiFe démontrent une activité et une stabilité exceptionnelles résultant d'une structure originale cœur-coquille-coquille générée in situ, tandis que les nanoparticules de CoSi riches en défauts présentent un ferromagnétisme inhabituel. De plus, l'étude des nanoparticules de silicophosphure donne un aperçu de la conception de matériaux multinaires dans les sels fondus et du rôle des éléments non métalliques dans l’électrocatalyse de l’électrolyse de l’eau
Transition metal silicides are a family of intermetallic compounds, which have been widely studied as functional materials in integrated circuits, thermoelectricity, superconductivity, magnetism and heterogeneous catalysis. Nanostructuration offers the opportunity to extend the frontier of silicon-based materials science with novel phases and diverse properties. However, building transition metal silicides encompassing relatively high energy bonds usually requires high temperatures, which are not conducive for nanomaterial design and not compatible with the traditional colloidal synthesis methods. In this thesis, molten salts syntheses based on element insertion into nanoparticles are developed. Transition metal silicide nanoparticles (M-Si, M=Ni, Fe, NiFe, Co) and a ternary nickel silicophosphide are crystallized in high temperature inorganic solvents, where a diluted and carbon-free environment is provided. The obtained silicide nanoparticles are investigated in electrocatalysis of alkaline water oxidation and magnetism. NiFe silicides demonstrate outstanding activity and stability arising from an original in situ generated core-shell-shell structure, while defect-rich CoSi nanoparticles show an unusual surface related ferromagnetism. Moreover, the study of silicophosphide nanoparticles provides an insight in multinary material design in molten salts and the role of nonmetal elements in overall alkaline water splitting electrocatalysis

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Liu, Meng <1991&gt. „Nanocarbon-Supported Electrocatalysts for the Alkaline Water Splitting and Fuel Cells“. Doctoral thesis, Alma Mater Studiorum - Università di Bologna, 2021. http://amsdottorato.unibo.it/9544/1/Liu_Meng_thesis.pdf.

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Electrocatalysts play a significant role in the processes of electrochemical energy conversion. This thesis focuses on the preparation of carbon-supported nanomaterials and their application as electrocatalysts for alkaline water electrocatalysis and fuel cell. A general synthetic route was developed, i.e., species intercalate into carbon layers of graphite forming graphite intercalation compound, followed by dispersion producing graphenide solution, which then as reduction agent reacts with different metal sources generating the final materials. The first metal precursor used was non-noble metal iron salt, which generated iron (oxide) nanoparticles finely dispersed on carbon layers in the final composite materials. Meanwhile, graphite starting materials differing in carbon layer size were utilized, which would diversify corresponding graphenide solutions, and further produce various nanomaterials. The characterization results showed that iron (oxide) nanoparticles varying in size were obtained, and the size was determined by the starting graphite material. It was found that they were electrocatalytically active for oxygen reactions. In particular, the one with small iron (oxide) nanoparticles showed excellent electrocatalytic activity for both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Afterwards, the metal precursor was tuned from non-noble metal salt to noble metal salt. It was confirmed that carbon-supported Rh, Pt, and RhPt (oxide) nanoparticle composite materials were also successfully obtained from the reaction between graphenide solution and corresponding noble metal precursor. The electrochemical measurements showed that the prepared noble metal-based nanomaterials were quite effective for hydrogen evolution reaction (HER) electrocatalysis, and the Rh sample could also display excellent electrocatalytic property towards OER. Moreover, by this synthetic approach carbon-supported noble metal Pt and non-noble metal nickel (Ni) composite material was also prepared. Therefore, the utilization efficiency of noble metal could be improved. The prepared NiPt sample displayed a property close to benchmark HER electrocatalyst.

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Fan, Kaicai. „Development of High Performance Electrocatalyst for Water Splitting Application“. Thesis, Griffith University, 2018. http://hdl.handle.net/10072/382229.

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With increasing global demand for energy, rapid depletion of fossil fuels and intensification of environmental concerns, exploring clean and sustainable energy carriers to replace fossil fuel is becoming critical. Among the various alternatives, hydrogen has been intensively regarded as a promising energy carrier to fulfill the increasing energy demand due to its large energy density per unit mass and eco-friendly production possibilities. However, hydrogen does not exist in molecular structure in nature, and it is essential to obtain efficient and sustainable H2 production technologies. Alkaline water electrolysis is an effective, clean and sustainable process to produce high-quality hydrogen. In this process, highly active electrocatalysts for the hydrogen evolution reaction (HER) are required to accelerate the sluggish kinetics and lower the overpotentials (η) for efficient hydrogen evolution. To date, a noble metal, platinum (Pt), is the state-of-art electrocatalyst for HER. However, exploration of alternative electrocatalysts with low cost and excellent electrocatalytic activity is of vital importance to realize large-scale hydrogen production through water electrolysis. Generally, an electrochemically active catalyst should have an optimal hydrogen adsorption free energy to allow efficient catalytic hydrogen adsorption/desorption. In alkaline solution, dissociation of water onto the electrocatalyst determines the overall HER efficiency. This thesis focuses on rational design and synthesis of different earth-abundant electrocatalysts for electrocatalytic HER in alkaline media. Through facile anion or cation doping strategies, electrocatalysts with abundant accessible active sites, enhanced electronic conductivity and accelerated HER kinetics have been systematically fabricated, characterized and evaluated. First, an efficient HER electrocatalyst in alkaline media was fabricated by incorporating sulfur atoms into a cobalt (hydro)oxide crystal structure. The resultant catalyst exhibits a remarkably enhanced HER activity with a low-overpotential of 119 mV at 10 mA/cm2 and an excellent durability. The results suggest that cobalt hydroxide benefits water adsorption and cleavage, while the negatively charged sulfur ligands facilitate hydrogen adsorption and desorption on the surface of electrocatalysts, leading to significantly promoted Volmer and Heyrovsky steps for HER in alkaline media. Second, exploring bifunctional electrocatalysts which can simultaneously accelerate the HER and oxygen evolution reaction (OER) activities plays a key role in alkaline water splitting. Here, sulfur atoms were incorporated into the mixed transition metal hydroxide with high OER performance to render excellent HER activity. The enhanced catalytic activity towards HER was confirmed by a synergistic effect between the retained metal hydroxide host and the incorporated sulfur atoms. In addition, the full water splitting electrolyzer equipped with fabricated bifunctional electrocatalysts as anode and cathode materials exhibited remarkable overall water splitting performance comparable to that with benchmark Pt and RuO2 electrocatalysts. The S/Se co-doped Co3O4 nanosheets on carbon cloth were fabricated by a facile room temperature chalcogen atom incorporation methodology and were applied as the electrocatalyst for HER in alkaline media. The sulfur and selenium atoms were homogeneously distributed on the surface by forming Co-S or Co-Se bonds which play a key role in the structural change in electrochemical activation. The obtained electrocatalysts demonstrated remarkably improved HER activity compared to that of the original Co3O4. Finally, molybdenum doped cobalt hydroxide was fabricated with significantly accelerated HER kinetics. The introduced Mo sites not only effectively facilitate water dissociation process and desorption of the OHads intermediates, but also simultaneously optimize the hydrogen adsorption free energy. Therefore, the in situ-generated Mo-doped amorphous cobalt hydroxide exhibited a remarkable HER performance in alkaline media with an overpotential of only -80 mV at a current density of 10 mA/cm2. This thesis innovatively explores strategies to improve the catalytic activity towards HER of metal (hydro)oxide in alkaline media. The surface foreign atom doping was demonstrated to manipulate the surface structure of catalysts, thus not only improving the water dissociation processes, but also facilitating the hydrogen adsorption/desorption on the catalysts. The demonstrated facile and effective strategies could be adopted for the fabrication of cost-effective and highly active catalysts for other important chemical reactions for energy conversion applications.
Thesis (PhD Doctorate)
Doctor of Philosophy (PhD)
School of Environment and Sc
Science, Environment, Engineering and Technology
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Zhang, Jian, Tao Wang, Darius Pohl, Bernd Rellinghaus, Renhao Dong, Shaohua Liu, Xiaodong Zhuang und Xinliang Feng. „Interface Engineering of MoS2/Ni3S2 Heterostructures for Highly Enhanced Electrochemical Overall Water Splitting Activity“. Saechsische Landesbibliothek- Staats- und Universitaetsbibliothek Dresden, 2018. http://nbn-resolving.de/urn:nbn:de:bsz:14-qucosa-235457.

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To achieve sustainable production of H2 fuel through water splitting, low-cost electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) are required to replace Pt and IrO2 catalysts. Here, for the first time, we present the interface engineering of novel MoS2/Ni3S2 heterostructures, in which abundant interfaces are formed. For OER, such MoS2/Ni3S2 heterostructures show an extremely low overpotential of ~218 mV at 10 mA cm-2, which is superior to that of the state-of-the-art OER electrocatalysts. Using MoS2/Ni3S2 heterostructures as bifunctional electrocatalysts, an alkali electrolyser delivers a current density of 10 mA cm-2 at a very low cell voltage of ~1.56 V. In combination with density function theory (DFT) calculations, this study demonstrates that the constructed interfaces synergistically favor the chemisorption of hydrogen and oxygencontaining intermediates, thus accelerating the overall electrochemical water splitting.

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Park, Kyoung-Won. „Solar-driven overall water splitting on CoO nanoparticles : first-principles density functional theory studies“. Thesis, Massachusetts Institute of Technology, 2018. http://hdl.handle.net/1721.1/117802.

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Thesis: Ph. D., Massachusetts Institute of Technology, Department of Materials Science and Engineering, 2018.
This electronic version was submitted by the student author. The certified thesis is available in the Institute Archives and Special Collections.
Cataloged student-submitted from PDF version of thesis.
Includes bibliographical references (pages 143-157).
Photoelectrochemical (PEC) water splitting has been suggested as a promising techinique for large-scale hydrogen fuel production. In particular, spontaneous photocatalytic overall water splitting on self-standing particles in water without external driving potential has been highlighted as a clean and economical energy generation method for the future. Among various photocatalytic materials, some cobalt-based materials including CoP, Co₂P, Co(OH)₂, CoO, have attained major interest because they exhibit improved catalytic activity for hydrogen evolution in the form of nanoparticles, unlike most cobalt-based materials which have been assessed as water oxidizing catalysts in the past decade. CoO nanoparticles have been observed to photocatalytically split water into H₂ and O₂ at room temperature without an externally applied potential or co-catalyst, with high photo-catalytic efficiency (solar-to-hydrogen efficiency of ~5%) which hits the record among single-material self-standing photocatalysts. The photocatalytic activity of CoO nanoparticles was experimentally shown to stem from the optimal conduction and valence band edge positions (Ec and Ev) relative to water reduction and oxidation potential levels (H+/H₂ and H₂O/O₂), such that the Ec and EV span the water redox potentials. The overall water splitting is not expected from CoO micropowder or bulk CoO because they have band edges far below the H+/H2 level, which are not optimal for overall water splitting. However, the origin of the shift in the band edges due to decrease in particle size (from bulk or micropowder to nanoparticle) was unknown. Moreover, the mechanism by which H₂ and O₂ simultaneously and spontaneously evolve on the nanoparticles, as well as how the CoO nanoparticles could exhibit a high photocatalytic efficiency even without a co-catalyst or an external driving potential have remained unanswered. In this work, we use first-principles density functional theory (DFT) calculations to explore thermodynamically stable surface configurations of CoO in an aqueous environment in which photocatalytic water splitting occurs. We also calculate the Ec and Ev of CoO surfaces relative to water redox potentials, showing that the band edge positions are sensitive to surface chemistry which is determined by surface orientation, adsorbates, and stoichiometry, and thus growth conditions and operating environment. In particular, we predict that CoO nanoparticles have fully hydroxylated CoO(111) facets (OH*-CoO(111)), with band edges spanning the water redox potentials, while larger CoO particles (such as CoO micropowders) have a full monolayer of hydrogen on the CoO(111) facets, with a band alignment that favors water oxidation but not water reduction. From these calculations, we demonstrate that explicit inclusion of liquid water is crucial for accurately predicting the band edge positions, and thus photocatalytic behavior of CoO in an aqueous solution. In order to find the origin of the high efficiency and spontaneous overall water splitting without an external bias or a co-catalyst, we also elucidate the mechanisms for charge separation and H₂ and O₂ evolution on CoO nanoparticles under illumination in an aqueous solution. We demonstrate that electrons are driven to CoO(100) facets and holes are driven to OH*-CoO(111) facets as a result of a built-in potential arising from the very different potential levels of the two facets. We show that H₂ evolution preferentially occurs on the CoO(100) facets, while O2 evolves on the OH*-CoO(111) surfaces, based on our new criteria. Importantly, we suggest that the conventional criterion for determining the feasibility of H₂ or O₂ generation from water splitting - i.e., EC < H+/H₂ level or Ev > H₂O/O₂ level - is insufficient. Instead, we suggest that a more appropriate set of criteria is whether the photo-excited electrons and holes have sufficient energy to overcome the kinetic barrier for the H₂ and O₂ evolution reaction, respectively, on the relevant surface facet. This work explains why and how photocatalytic overall water splitting has been observed only on CoO nanoparticles. Our understanding of the overall water splitting mechanism on CoO nanoparticles provides a general explanation of experimentally observed overall water splitting phenomena on a variety of self-standing photocatalysts as well as a new approach for screening novel photocatalytic materials for efficient water splitting and other reactions.
by Kyoung-Won Park.
Ph. D.

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Adeli, Koudehi Babak. „Solar hydrogen generation through overall water splitting on gallium-zinc oxynitride visible-light activated photocatalyst“. Thesis, University of British Columbia, 2017. http://hdl.handle.net/2429/60303.

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In this study, novel approaches for the development of solar-responsive photocatalysts for water splitting are investigated, with a focus on the gallium-zinc oxynitride solid solution (GaN:ZnO). A facile synthesis technique was developed for the fabrication of nanoporous GaN:ZnO photocatalyst. The synthesis time was reduced substantially to 12 min (from original 10+ h) as the result of effective solid–solid and gas–solid reactant interactions at the nanoscale. The synthesized photocatalyst samples were characterized for their optical, structural, and photochemical properties. Despite the short synthesis time, the prepared nanoporous GaN:ZnO photocatalyst maintained the overall visible-light water splitting activities at reasonable rates, reaching to the maximum apparent quantum efficiency of 2.71% at 420–440 nm. Decoration of the photocatalyst surface with the optimal amount of various hydrogen and oxygen evolution co-catalyst materials through photo-deposition and impregnation was investigated. Our experimental and characterization data suggest a mechanism for minimizing the effect of the undesired charge recombination and reverse reaction through the utilization of structural nanopores as the active water splitting regions. To reduce the recombination of photo-excited charges, the hybridization of GaN:ZnO photocatalyst on highly conductive graphene support was studied. Effective electrochemical interaction between composite components was confirmed through material characterization, photo-induced conversion of graphene oxide to reduced graphene oxide (rGO), and visual observation of co-catalyst nanoparticles on the surface of the conductive nanosheets. The GaN:ZnO-rGO composite photocatalyst exhibited ~70% improvement in photocatalytic hydrogen evolution. Finally, a number of approaches for the synthesis of one-dimensional (1-D) GaN:ZnO photocatalysts were studied. A novel direct fabrication route for 1-D GaN:ZnO through gold-catalyzed atmospheric pressure chemical vapour deposition was proposed. The material characterization data indicated that the proposed method is capable of preparing 1-D GaN:ZnO nanostructures with a wide range of morphologies, including nanofibers and nanowires, via vapour–liquid–solid epitaxy. In addition, via the proposed method, the dimensions of the obtained nanomaterials can be tailored. The synthesized GaN:ZnO nanowires demonstrated promising sacrificial hydrogen evolution compared to the powder and nanofiber photocatalysts. The work presented in this research provides an in-depth understanding of the nanoscale fabrication and optimization of GaN:ZnO photocatalysts for visible-light hydrogen generation.
Chemical and Biological Engineering, Department of
Graduate

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Li, Junwei. „Investigation of Structural-Catalytic Relationship of Mixed-Metal Layered Oxide Materials for Photocatalytic Overall Water Splitting“. Thesis, The University of Sydney, 2022. https://hdl.handle.net/2123/29385.

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Hydrogen can be generated renewably by sunlight driven, photocatalytic water splitting. Metal oxides, including those with a Ruddlesden-Popper type structures are being studied as potential photocatalysts. From the initial testing of multiple metal oxides, KLaTiO4 and Na3Co2SbO6 was found to be particularly effective as catalyst for hydrogen evolution. During testing, the solid-state synthesis of KLaTiO4 was found to be unreliable, with most samples found with K2La2Ti3O10 impurities. Two main factors were found to have significantly impacted the yield of KLaTiO4. The first factor to consider is the volatility of alkali metal ions at elevated temperatures. Successful synthesis of KLaTiO4 required 50 % (minimum tested) alkali metal reagent excess. The second factor to consider is related to sintering temperature. From the results of the synthetic experiments, the ideal heating temperature of KLaTiO4 is 800 °C, and the ideal heating temperature of K2La2Ti3O10 is850 °C, which is lower than other literature reports. As a Hydrogen Evolution Catalyst (HEC), the main disadvantage of KLaTiO4 is its high bandgap of 4.09(13) eV. To reduce the bandgap of KLaTiO4, both cationic and anionic doping of the sample is attempted. Cationic doping of KLaTiO4 was achieved by partially replacing lanthanum with ytterbium, yielding KLa1-xYbxTiO4 (x = 0.005, 0.01 and 0.03). In comparison to KLaTiO4, ytterbium doped samples have a reduced catalytic activity compared to the undoped sample. Anionic doping of KLaTiO4 was attempted by nitrogen doping using TiN as a reagent in place of TiO2, and have the sample annealed under N2 flow, at 800 °C, yielding KLaTiO3N. KLaTiO3N shows good crystallinity, and no observable structural difference to KLaTiO4. When tested as HEC in identical testing condition, KLaTiO3N had a third rate of hydrogen evolution in comparison to KLaTiO4.

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Berto, Tobias [Verfasser], Johannes A. [Akademischer Betreuer] [Gutachter] Lercher und Tom [Gutachter] Nilges. „Elucidation of reaction pathways of the photoreforming and overall water splitting reaction over precious metal decorated semiconductors / Tobias Berto ; Gutachter: Johannes A. Lercher, Tom Nilges ; Betreuer: Johannes A. Lercher“. München : Universitätsbibliothek der TU München, 2016. http://d-nb.info/1123210861/34.

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Buchteile zum Thema "Overall alkaline water splitting"

Shit, Subhasis, Tapas Kuila und Suneel Kumar Srivastava. „Noble-Metal-Free Bifunctional Electrocatalysts for Overall Water Splitting in Alkaline Medium“. In Advances in Catalysts Research, 279–337. Cham: Springer Nature Switzerland, 2024. http://dx.doi.org/10.1007/978-3-031-49108-5_9.

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Peng, Shengjie. „Alkaline Water Electrolysis“. In Electrochemical Hydrogen Production from Water Splitting, 57–68. Singapore: Springer Nature Singapore, 2023. http://dx.doi.org/10.1007/978-981-99-4468-2_3.

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Karuppasamy, Lakshmanan, Lakshmanan Gurusamy und Jerry J. Wu. „Nanocomposites for Overall Water-Splitting“. In Handbook of Energy Materials, 1–31. Singapore: Springer Nature Singapore, 2022. http://dx.doi.org/10.1007/978-981-16-4480-1_73-1.

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Yang, Yang. „Bifunctional Electrocatalysts for Overall Water Splitting“. In Electrochemical Transformation of Renewable Compounds, 4–37. Boca Raton: CRC Press, 2022. http://dx.doi.org/10.1201/9780429326783-2.

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Ertekin, Zeliha, und Demet Ozer. „2D Materials for Overall Water Splitting“. In Handbook of Energy Materials, 1–26. Singapore: Springer Nature Singapore, 2022. http://dx.doi.org/10.1007/978-981-16-4480-1_72-1.

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Martin, David James. „Novel Z-Scheme Overall Water Splitting Systems“. In Springer Theses, 123–43. Cham: Springer International Publishing, 2015. http://dx.doi.org/10.1007/978-3-319-18488-3_5.

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Li, Shasha, Enze Li, Caixia Shi, Yuanyang Wang, Yongbin Xue, Xiaowei An und Guoqing Guan. „Metal Oxides and Sulfides for Overall Water Splitting“. In Handbook of Energy Materials, 1–28. Singapore: Springer Nature Singapore, 2022. http://dx.doi.org/10.1007/978-981-16-4480-1_45-1.

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Townsend, Troy K., Nigel Browning und Frank E. Osterloh. „Overall Photocatalytic Water Splitting with Suspended NiO-SrTiO3 Nanocrystals“. In Inorganic Metal Oxide Nanocrystal Photocatalysts for Solar Fuel Generation from Water, 39–51. Cham: Springer International Publishing, 2014. http://dx.doi.org/10.1007/978-3-319-05242-7_4.

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Sharafinia, Soheila, und Alimorad Rashidi. „One-Dimensional Polymeric Nanocomposites for Overall Water-Splitting Applications“. In One-Dimensional Polymeric Nanocomposites, 231–54. Boca Raton: CRC Press, 2022. http://dx.doi.org/10.1201/9781003223764-13.

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Bhagat, Devidas S., Gurvinder S. Bumbrah und Wasudeo B. Gurnule. „Rare Earth Element Based Functionalized Electrocatalysts in Overall Water Splitting Reactions“. In Energy, Environment, and Sustainability, 205–18. Singapore: Springer Singapore, 2022. http://dx.doi.org/10.1007/978-981-16-8599-6_9.

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Konferenzberichte zum Thema "Overall alkaline water splitting"

„CoMo2S4/MoS2 Heterostructure with High Catalytic Performance for Overall Water Splitting in Alkaline Medium“. In 2018 International Conference on Medicine, Biology, Materials and Manufacturing. Francis Academic Press, 2018. http://dx.doi.org/10.25236/icmbmm.2018.47.

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Albornoz, Matias, Marco Rivera, Roberto Ramirez, Felipe Varas-Concha und Patrick Wheeler. „Water Splitting Dynamics of High Voltage Pulsed Alkaline Electrolysis“. In 2022 IEEE International Conference on Automation/XXV Congress of the Chilean Association of Automatic Control (ICA-ACCA). IEEE, 2022. http://dx.doi.org/10.1109/ica-acca56767.2022.10006326.

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Domen, Kazunari. „Overall water splitting on (oxy)nitride photocatalysts“. In Solar Energy + Applications, herausgegeben von Gunnar Westin. SPIE, 2008. http://dx.doi.org/10.1117/12.798334.

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Longo, Filippo, Emanuel Billeter, Zbynek Novotny und Andreas Borgschulte. „Nickel Surface Modifications upon O2/H2O Oxidation and Alkaline Water Splitting“. In International Conference on Frontiers in Electrocatalytic Transformations. València: FUNDACIO DE LA COMUNITAT VALENCIANA SCITO, 2022. http://dx.doi.org/10.29363/nanoge.interect.2022.013.

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Hisatomi, Takashi, und Kazunari Domen. „Recent progress in photocatalysts for overall water splitting under visible light“. In SPIE Solar Energy + Technology, herausgegeben von Frank E. Osterloh. SPIE, 2009. http://dx.doi.org/10.1117/12.829992.

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Kibria, M. G., F. A. Chowdhury, H. P. T. Nguyen, S. Zhao und Z. Mi. „Overall Water Splitting under Broadband Light Using InGaN/GaN Nanowire Heterostructures“. In 2014 IEEE Photonics Society Summer Topical Meeting Series. IEEE, 2014. http://dx.doi.org/10.1109/sum.2014.17.

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Wang, Lili, Helin Zhang, Wurigamula He, Qianli Ma, Wensheng Yu, Shuang Gao, Da Xu, Duanduan Yin und Xiangting Dong. „Hierarchical NiFe layered double hydroxides: a bifunctional electrocatalyst for overall water splitting“. In 2021 IEEE International Conference on Manipulation, Manufacturing and Measurement on the Nanoscale (3M-NANO). IEEE, 2021. http://dx.doi.org/10.1109/3m-nano49087.2021.9599799.

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Thennarasi, A., und Kuraganti Vasu. „Synthesis of electrocatalytic active bifunctional Fe-doped MoS2 nanosheets for overall water splitting“. In 66TH DAE SOLID STATE PHYSICS SYMPOSIUM. AIP Publishing, 2024. http://dx.doi.org/10.1063/5.0178149.

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O’Brien, J. E. „Thermodynamic Considerations for Thermal Water Splitting Processes and High Temperature Electrolysis“. In ASME 2008 International Mechanical Engineering Congress and Exposition. ASMEDC, 2008. http://dx.doi.org/10.1115/imece2008-68880.

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A general thermodynamic analysis of hydrogen production based on thermal water splitting processes is presented. Results of the analysis show that the overall efficiency of any thermal water splitting process operating between two temperature limits is proportional to the Carnot efficiency. Implications of thermodynamic efficiency limits and the impacts of loss mechanisms and operating conditions are discussed as they pertain specifically to hydrogen production based on high-temperature electrolysis. Overall system performance predictions are also presented for high-temperature electrolysis plants powered by three different advanced nuclear reactor types, over their respective operating temperature ranges.

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Akasyah, Luqman, und Rajdeep Singh Rawat. „Plasma-Based Synthesis of Tritantalum Pentanitride for Visible-Light Driven Photocatalytic Overall Water Splitting“. In 2020 IEEE International Conference on Plasma Science (ICOPS). IEEE, 2020. http://dx.doi.org/10.1109/icops37625.2020.9717660.

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Berichte der Organisationen zum Thema "Overall alkaline water splitting"

Litaor, Iggy, James Ippolito, Iris Zohar und Michael Massey. Phosphorus capture recycling and utilization for sustainable agriculture using Al/organic composite water treatment residuals. United States Department of Agriculture, Januar 2015. http://dx.doi.org/10.32747/2015.7600037.bard.

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Objectives: 1) develop a thorough understanding of the sorption mechanisms of Pi and Po onto the Al/O- WTR; 2) determine the breakthrough range of the composite Al/O-WTR during P capturing from agro- wastewaters; and 3) critically evaluate the performance of the composite Al/O-WTR as a fertilizer using selected plants grown in lysimeters and test-field studies. Instead of lysimeters we used pots (Israel) and one- liter cone-tainers (USA). We conducted one field study but in spite of major pretreatments the soils still exhibited high enough P from previous experiments so no differences between control and P additions were noticeable. Due to time constrains the field study was discontinued. Background: Phosphorous, a non-renewable resource, has been applied extensively in fields to increase crop yield, yet consequently has increased the potential of waterway eutrophication. Our proposal impetus is the need to develop an innovative method of P capturing, recycling and reuse that will sustain agricultural productivity while concurrently reducing the level of P discharge from and to agricultural settings. Major Conclusions & Achievements: An innovative approach was developed for P removal from soil leachate, dairy wastewater (Israel), and swine effluents (USA) using Al-based water treatment residuals (Al- WTR) to create an organic-Al-WTR composite (Al/O-WTR), potentially capable of serving as a P fertilizer source. The Al-WTR removed 95% inorganic-P, 80% to 99.9% organic P, and over 60% dissolved organic carbon from the agro-industrial waste streams. Organic C accumulation on particles surfaces possibly enhanced weak P bonding and facilitated P desorption. Analysis by scanning electron microscope (SEM- EDS), indicated that P was sparsely sorbed on both calcic and Al (hydr)oxide surfaces. Sorption of P onto WW-Al/O-WTR was reversible due to weak Ca-P and Al-P bonds induced by the slight alkaline nature and in the presence of organic moieties. Synchrotron-based microfocused X-ray fluorescence (micro-XRF) spectrometry, bulk P K-edge X-ray absorption near edge structure spectroscopy (XANES), and P K-edge micro-XANES spectroscopy indicated that adsorption was the primary P retention mechanism in the Al- WTR materials. However, distinct apatite- or octocalciumphosphatelike P grains were also observed. Synchrotron micro-XRF mapping further suggested that exposure of the aggregate exteriors to wastewater caused P to diffuse into the porous Al-WTR aggregates. Organic P species were not explicitly identified via P K-edge XANES despite high organic matter content, suggesting that organic P may have been predominantly associated with mineral surfaces. In screen houses experiments (Israel) we showed that the highest additions of Al/O-WTR (5 and 7 g kg⁻¹) produced the highest lettuce (Lactuca sativa L. var. longifolial) yield. Lettuce yield and P concentration were similar across treatments, indicating that Al/O- WTR can provide sufficient P to perform similarly to common fertilizers. A greenhouse study (USA) was utilized to compare increasing rates of swine wastewater derived Al/O-WTR and inorganic P fertilizer (both applied at 33.6, 67.3, and 134.5 kg P₂O₅ ha⁻¹) to supply plant-available P to spring wheat (TriticumaestivumL.) in either sandy loam or sandy clay loam soil. Spring wheat straw and grain P uptake were comparable across all treatments in the sandy loam, while Al/O-WTR application to the sandy clay loam reduced straw and grain P uptake. The Al/O-WTR did not affect soil organic P concentrations, but did increase phosphatase activity in both soils; this suggests that Al/O-WTR application stimulated microorganisms and enhance the extent to which microbial communities can mineralize Al/O-WTR-bound organic P. Implications: Overall, results suggest that creating a new P fertilizer from Al-WTR and agro-industrial waste sources may be a feasible alternative to mining inorganic P fertilizer sources, while protecting the environment from unnecessary waste disposal.

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Clark, Donald L., Stefan M. Kirby und Charles G. Oviatt. Geologic Map of the Rush Valley 30' X 60' Quadrangle, Tooele, Utah, and Salt Lake Counties, Utah. Utah Geological Survey, August 2023. http://dx.doi.org/10.34191/m-294dm.

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The Rush Valley 30' x 60' quadrangle extends southwest and west from the greater Salt Lake City–Provo metropolitan area with land use varied between public, military, Indian reservation, and private. This 1:62,500-scale geologic map will aid the proper management of land, water, and other resources. The map area lies within the eastern Basin and Range Province. Mountain ranges are composed of unexposed basement rocks overlain by exposed Neoproterozoic through Triassic rocks that are about 10.4 miles (16.8 km) thick, and by numerous Tertiary sedimentary and volcanic units (~47 to 20 Ma). The intervening valleys include bedrock covered with Miocene-Pliocene? rocks (~11 to 4 Ma) and Neogene-Quaternary surficial deposits. The map area is on the southern flank of the Uinta-Tooele structural zone. This area is in the Charleston-Nebo (Provo) salient of the Sevier fold-thrust belt and some thrust faults are exposed, but the overall Sevier belt geometry is obscured by extensive Cenozoic cover and later faulting. Following Sevier deformation, calk-alkaline volcanism occurred from several Paleogene volcanic centers (42 to 25 Ma). Extensional tectonism created the distinctive basin and range topography from about 20 Ma to the present. Early extensional basin fill includes Miocene sedimentary and volcanic rocks followed by Pliocene-Holocene surficial deposits primarily from lacustrine and alluvial depositional environments. Valley areas were covered by late Pleistocene Lake Bonneville, and deposits are associated with three levels of regional shorelines. Normal faults cut the ranges and are known to bound some valley margins where not concealed. Although deep drill hole data are relatively sparse, gravity data were used to help constrain basin geometries.

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