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Journal articles on the topic 'Semi-Heterogeneous Lewis Frustrated Pair'

Author: Grafiati
Published: 25 May 2024

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1

Ma, Yuanyuan, Sai Zhang, Chun-Ran Chang, Zheng-Qing Huang, Johnny C. Ho, and Yongquan Qu. "Semi-solid and solid frustrated Lewis pair catalysts." Chemical Society Reviews 47, no. 15 (2018): 5541–53. http://dx.doi.org/10.1039/c7cs00691h.

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2

Wan, Qiang, Sen Lin, and Hua Guo. "Frustrated Lewis Pairs in Heterogeneous Catalysis: Theoretical Insights." Molecules 27, no. 12 (June 10, 2022): 3734. http://dx.doi.org/10.3390/molecules27123734.

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Frustrated Lewis pair (FLP) catalysts have attracted much recent interest because of their exceptional ability to activate small molecules in homogeneous catalysis. In the past ten years, this unique catalysis concept has been extended to heterogeneous catalysis, with much success. Herein, we review the recent theoretical advances in understanding FLP-based heterogeneous catalysis in several applications, including metal oxides, functionalized surfaces, and two-dimensional materials. A better understanding of the details of the catalytic mechanism can help in the experimental design of novel heterogeneous FLP catalysts.
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3

Liu, Lei, Jan Gerit Brandenburg, and Stefan Grimme. "On the hydrogen activation by frustrated Lewis pairs in the solid state: benchmark studies and theoretical insights." Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences 375, no. 2101 (July 24, 2017): 20170006. http://dx.doi.org/10.1098/rsta.2017.0006.

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Recently, the concept of small molecule activation by frustrated Lewis pairs (FLPs) has been expanded to the solid state showing a variety of interesting reactivities. Therefore, there is a need to establish a computational protocol to investigate such systems theoretically. In the present study, we selected several FLPs and applied multiple levels of theory, ranging from a semi-empirical tight-binding Hamiltonian to dispersion corrected hybrid density functionals. Their performance is benchmarked for the computation of crystal geometries, thermostatistical contributions, and reaction energies. We show that the computationally efficient HF-3c method gives accurate crystal structures and is numerically stable and sufficiently fast for routine applications. This method also gives reliable values for the thermostatistical contributions to Gibbs free energies. The meta-generalized gradient approximated TPSS-D3 evaluated in a projector augmented plane wave basis set is able to produce sufficiently accurate reaction electronic energies. The established protocol is intended to support experimental studies and to predict new reactions in the emerging field of solid-state FLPs. This article is part of the themed issue ‘Frustrated Lewis pair chemistry’.
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4

Ghuman, Kulbir Kaur, Laura B. Hoch, Paul Szymanski, Joel Y. Y. Loh, Nazir P. Kherani, Mostafa A. El-Sayed, Geoffrey A. Ozin, and Chandra Veer Singh. "Photoexcited Surface Frustrated Lewis Pairs for Heterogeneous Photocatalytic CO2 Reduction." Journal of the American Chemical Society 138, no. 4 (January 25, 2016): 1206–14. http://dx.doi.org/10.1021/jacs.5b10179.

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5

Ghuman, Kulbir Kaur, Laura B. Hoch, Thomas E. Wood, Charles Mims, Chandra Veer Singh, and Geoffrey A. Ozin. "Surface Analogues of Molecular Frustrated Lewis Pairs in Heterogeneous CO2 Hydrogenation Catalysis." ACS Catalysis 6, no. 9 (August 2, 2016): 5764–70. http://dx.doi.org/10.1021/acscatal.6b01015.

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6

Trunk, Matthias, Johannes F. Teichert, and Arne Thomas. "Room-Temperature Activation of Hydrogen by Semi-immobilized Frustrated Lewis Pairs in Microporous Polymer Networks." Journal of the American Chemical Society 139, no. 10 (March 3, 2017): 3615–18. http://dx.doi.org/10.1021/jacs.6b13147.

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7

Liu, Qiang, Qiaobo Liao, Jinling Hu, Kai Xi, Youting Wu, and Xingbang Hu. "Covalent organic frameworks anchored with frustrated Lewis pairs for hydrogenation of alkynes with H2." Journal of Materials Chemistry A 10, no. 13 (2022): 7333–40. http://dx.doi.org/10.1039/d1ta08916a.

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8

Ghoussoub, Mireille, Shwetank Yadav, Kulbir Kaur Ghuman, Geoffrey A. Ozin, and Chandra Veer Singh. "Metadynamics-Biased ab Initio Molecular Dynamics Study of Heterogeneous CO2 Reduction via Surface Frustrated Lewis Pairs." ACS Catalysis 6, no. 10 (September 23, 2016): 7109–17. http://dx.doi.org/10.1021/acscatal.6b01545.

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9

Niu, Zheng, Weijie Zhang, Pui Ching Lan, Briana Aguila, and Shengqian Ma. "Promoting Frustrated Lewis Pairs for Heterogeneous Chemoselective Hydrogenation via the Tailored Pore Environment within Metal–Organic Frameworks." Angewandte Chemie International Edition 58, no. 22 (May 27, 2019): 7420–24. http://dx.doi.org/10.1002/anie.201903763.

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10

Niu, Zheng, Weijie Zhang, Pui Ching Lan, Briana Aguila, and Shengqian Ma. "Promoting Frustrated Lewis Pairs for Heterogeneous Chemoselective Hydrogenation via the Tailored Pore Environment within Metal–Organic Frameworks." Angewandte Chemie 131, no. 22 (April 17, 2019): 7498–502. http://dx.doi.org/10.1002/ange.201903763.

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11

Dong, Yuchan, Kulbir Kaur Ghuman, Radian Popescu, Paul N. Duchesne, Wenjie Zhou, Joel Y. Y. Loh, Abdinoor A. Jelle, et al. "Tailoring Surface Frustrated Lewis Pairs of In2 O3− x (OH)y for Gas-Phase Heterogeneous Photocatalytic Reduction of CO2 by Isomorphous Substitution of In3+ with Bi3+." Advanced Science 5, no. 6 (March 12, 2018): 1700732. http://dx.doi.org/10.1002/advs.201700732.

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12

Dong, Yuchan, Kulbir Kaur Ghuman, Radian Popescu, Paul N. Duchesne, Wenjie Zhou, Joel Y. Y. Loh, Abdinoor A. Jelle, et al. "Solar Fuels: Tailoring Surface Frustrated Lewis Pairs of In2 O3− x (OH)y for Gas-Phase Heterogeneous Photocatalytic Reduction of CO2 by Isomorphous Substitution of In3+ with Bi3+ (Adv. Sci. 6/2018)." Advanced Science 5, no. 6 (June 2018): 1870034. http://dx.doi.org/10.1002/advs.201870034.

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13

Liu, Shulin, Minghua Dong, Yuxuan Wu, Sen Luan, Yu Xin, Juan Du, Shaopeng Li, Huizhen Liu, and Buxing Han. "Solid surface frustrated Lewis pair constructed on layered AlOOH for hydrogenation reaction." Nature Communications 13, no. 1 (April 28, 2022). http://dx.doi.org/10.1038/s41467-022-29970-6.

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AbstractDesigning heterogeneous solid surface frustrated Lewis pair (ssFLP) catalyst for hydrogenation is a new challenge in catalysis and no research has been reported on the construction of ssFLP on boehmite (AlOOH) surfaces up to now as far as we know. Herein, AlOOH with a layer structure is prepared and it is found that the Lewis basic OHv site (one H removed from OH) and an adjacent Lewis acidic unsaturated Al site (Al3+unsatur.) proximal to a surface OHv (OH vacancy) on AlOOH layers could form the ssFLP. The layered structure of AlOOH and its abundant OH defects over the surface result in a high concentration of OHv/Al3+unsatur. FLPs, which are conducive to highly efficient hydrogen activation for hydrogenation of olefins and alkynes with low H-H bond dissociates activation energy of 0.16 eV under mild conditions (T = 80°C and P(H2) = 2.0 MPa). This work develops a new kind of hydrogenation catalyst and provides a new perspective for creating solid surface FLP.
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14

Zhu, Yijia, Changping Jian, Ruifang Xue, Wei Zhang, Rou Guo, Yijing Gao, De-Li Chen, Fumin Zhang, Weidong Zhu, and Fang-Fang Wang. "Theoretical understanding on all-solid frustrated Lewis pair sites of C2N anchored by single metal atom." Journal of Chemical Physics, July 11, 2022. http://dx.doi.org/10.1063/5.0100170.

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Designing all-solid heterogeneous catalysts with frustrated Lewis pairs (FLPs) has aroused great attentions recently because of its appealing low dissociation energy for H2 molecule and thus a promotion of hydrogenation reaction is expected. The sterically encumbered Lewis acid (metal site) and base (nitrogen site) in the cavity of single transition metal atom doped M/C2N sheet makes it potential candidate with FLP, while a comprehensive understanding of its intrinsic property and reactivity is still required. Calculations show that the complete dissociation of H2 molecule into two H* at the N sites requires two steps, i.e., heterolytic cleavage of H2 molecule and the transfer of H* from metal site to N site, which are highly related to the acidity of the metal site. The Ni/C2N and Pd/C2N, which outperform over the other 8 transition metal atom (M) anchored M/C2N candidates, possess low energy barriers for the complete dissociation of H2 molecule, with values of only 0.30 and 0.20 eV, respectively. Furthermore, both Ni/C2N and Pd/C2N catalysts can achieve semi-hydrogenation of C2H2 into C2H4, with overall barriers of 0.81 and 0.75 eV, respectively, lower than many reported catalysts. It is speculated that M/C2N catalysts with intrinsic FLPs may also find applications in other important hydrogenation reaction.
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15

Zhang, Yin, Jun Guo, Peter VanNatta, Yao Jiang, Joshua Phipps, Roknuzzaman Roknuzzaman, Hassan Rabaâ, Kui Tan, Thamraa AlShahrani, and Shengqian Ma. "Metal-Free Heterogeneous Asymmetric Hydrogenation of Olefins Promoted by Chiral Frustrated Lewis Pair Framework." Journal of the American Chemical Society, December 20, 2023. http://dx.doi.org/10.1021/jacs.3c11607.

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16

Lu, Youluan, Haonan Wu, Dongna Li, Yi Huang, Huijuan Guo, Tielin Wang, Lijuan Shi, and Qun Yi. "De novo assembly of frustrated Lewis pair bearing metal‐organic frameworks for atmospheric CO2 cycloaddition." AIChE Journal, December 22, 2023. http://dx.doi.org/10.1002/aic.18349.

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AbstractPorous frustrated Lewis pairs (FLPs) have been demonstrated as cutting‐edge heterogeneous catalysts in acidic–basic catalysis, which, yet faces great challenges in synthesis. Herein, we propose a one‐step de novo assembly strategy for constructing porous FLPs by capping monodentate ionic liquids (ILs) on metal clusters during the synthesis of metal–organic frameworks (MOFs). The capping of ILs makes adjacent metal sites on MOFs transforming to coordinatively‐unsaturated metal Lewis acids, producing FLPs containing Lewis basic Cl− ions from ILs and metal sites. The distribution of ILs on the framework of MOFs endows the catalysts with large surface areas (up to 2125 m2 g−1), open channels and good stability. The porous FLPs behave unprecedented activity for atmospheric CO2 activation and coupling with epoxides (25–40°C, 1 bar, without cocatalyst). This de novo assembly strategy exhibits good universality for synthesizing porous FLPs from different kinds of ILs, paving a facile approach for designing high‐efficiency acidic–basic catalysts.
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17

Zhang, Yin, Songbo Chen, Abdullah M. Al-Enizi, Ayman Nafady, Zhiyong Tang, and Shengqian Ma. "Chiral Frustrated Lewis Pair@Metal‐Organic Framework as a New Platform for Heterogeneous Asymmetric Hydrogenation." Angewandte Chemie, November 8, 2022. http://dx.doi.org/10.1002/ange.202213399.

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18

Zhang, Yin, Songbo Chen, Abdullah M. Al-Enizi, Ayman Nafady, Zhiyong Tang, and Shengqian Ma. "Chiral Frustrated Lewis Pair@Metal‐Organic Framework as a New Platform for Heterogeneous Asymmetric Hydrogenation." Angewandte Chemie International Edition, November 8, 2022. http://dx.doi.org/10.1002/anie.202213399.

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19

Yao, Chang, Wenhua Li, Yurou Li, Yueqiang Cao, Jing Zhang, Gang Qian, Xinggui Zhou, and Xuezhi Duan. "Atomically dispersed Pt to boost adjacent frustrated Lewis pair for 2,6‐diamino‐3,5‐dinitropyridine hydrogenation." AIChE Journal, November 8, 2023. http://dx.doi.org/10.1002/aic.18278.

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AbstractAchieving atomic‐level control over local environment of metal oxide to boost catalytic activity is challenging yet significant for heterogeneous hydrogenations. Herein, we propose anchoring atomically dispersed Pt species onto indium oxide using a precisely conditioned atomic layer deposition (ALD) technology to manipulate the local electronic properties of In2O3 toward enhanced hydrogenation of 2,6‐diamino‐3,5‐dinitropyridine (DADNP) to 2,3,5,6‐tetraaminopyridine (TAP). Experimental and theoretical studies unravel that the isolated Pt atoms localize the electron density surrounding them and thus activate the adjacent frustrated Lewis pair for hydrogen activation. In addition, the adsorption of DADNP is enhanced by such regulation, while that of TAP is suppressed on the Pt1‐In2O3 catalyst. The as‐synthesized Pt1‐In2O3 catalyst thus exhibits 91.7% of TAP selectivity at 100% conversion of DADNP, demonstrating remarkably improved catalytic performances as compared with the In2O3 catalyst for DADNP hydrogenation.
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20

Zhang, Yin, Yao Jiang, Ayman Nafady, Zhiyong Tang, Abdullah M. Al-Enizi, Kui Tan, and Shengqian Ma. "Incorporation of Chiral Frustrated Lewis Pair into Metal–Organic Framework with Tailored Microenvironment for Heterogeneous Enantio- and Chemoselective Hydrogenation." ACS Central Science, July 27, 2023. http://dx.doi.org/10.1021/acscentsci.3c00637.

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21

Wu, Qingyuan, Ruixuan Qin, Mengsi Zhu, Hui Shen, Shenshui Yu, Yuanyua Zhong, Gang Fu, Xiaodong Yi, and Nanfeng Zheng. "Frustrated Lewis Pairs on Pentacoordinated Al3+-Enriched Al2O3 Promote Heterolytic Hydrogen Activation and Hydrogenation." Chemical Science, 2024. http://dx.doi.org/10.1039/d3sc06425e.

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As an emerging class of metal-free catalysts, frustrated Lewis pairs (FLPs) catalysts have been greatly constructed and applied in wide fields. Homogeneous FLPs have witnessed significant development, while limited heterogeneous...
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22

Chen, Miaomiao, Min Wang, and Min Ji. "Design and Synthesis of Heterogeneous Frustrated Lewis Pairs for Hydrogenation: From Molecular Immobilization to Defects Engineering." ChemCatChem, December 11, 2023. http://dx.doi.org/10.1002/cctc.202301472.

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The concept of “Frustrated Lewis pairs” (FLPs), which emerged from the discovery that H2 can be reversibly activated by combinations of sterically encumbered Lewis acids and bases. Since then, the field of FLP chemistry has expanded enormously. One of the most remarkable achievements is the development of FLP catalysts for hydrogenation, which are environmentally friendly and have potential industrial application prospects. In recent years, this unique catalysis concept has pushed the study of FLP chemistry to a new direction: heterogeneous FLP catalysts. This review outlines the recent research progress of new strategies to design and synthesize heterogeneous FLPs for hydrogenation reaction, and prospects the development of novel heterogeneous FLP catalysts.
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23

Du, Tao, Peng Zhang, Zhen Jiao, Jiancheng Zhou, and DING YUXIAO. "Homogeneous and Heterogeneous Frustrated Lewis Pairs for the Activation and Transformation of CO2." Chemistry – An Asian Journal, April 12, 2024. http://dx.doi.org/10.1002/asia.202400208.

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Due to the serious ecological problems caused by the high CO2 content in the atmosphere, reducing atmospheric CO2 has attracted widespread attention from academia and governments. Among the many ways to mitigate CO2 concentration, the capture and comprehensive utilization of CO2 through chemical methods have obvious advantages, whose key is to develop suitable adsorbents and catalysts. Frustrated Lewis pairs (FLPs) are known to bind CO2 through the interaction between unquenched Lewis acid sites/Lewis base sites with the O/C of CO2, simultaneously achieving CO2 capture and activation, which render FLP better potential for CO2 utilization. However, how to construct efficient FLP targeted for CO2 utilization and the mechanism of CO2 activation have not been systematically reported. This review firstly provides a comprehensive summary of the recent advances in the field of CO2 capture, activation, and transformation with the help of FLP, including the construction of homogeneous and heterogeneous FLPs, their interaction with CO2, reaction activity, and mechanism study. We also illustrated the challenges and opportunities faced in this field to shed light on the prospective research.
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24

Yan, Tingjiang, Na Li, Linlin Wang, Weiguang Ran, Paul N. Duchesne, Lili Wan, Nhat Truong Nguyen, Lu Wang, Meikun Xia, and Geoffrey A. Ozin. "Bismuth atom tailoring of indium oxide surface frustrated Lewis pairs boosts heterogeneous CO2 photocatalytic hydrogenation." Nature Communications 11, no. 1 (November 30, 2020). http://dx.doi.org/10.1038/s41467-020-19997-y.

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AbstractThe surface frustrated Lewis pairs (SFLPs) on defect-laden metal oxides provide catalytic sites to activate H2 and CO2 molecules and enable efficient gas-phase CO2 photocatalysis. Lattice engineering of metal oxides provides a useful strategy to tailor the reactivity of SFLPs. Herein, a one-step solvothermal synthesis is developed that enables isomorphic replacement of Lewis acidic site In3+ ions in In2O3 by single-site Bi3+ ions, thereby enhancing the propensity to activate CO2 molecules. The so-formed BixIn2-xO3 materials prove to be three orders of magnitude more photoactive for the reverse water gas shift reaction than In2O3 itself, while also exhibiting notable photoactivity towards methanol production. The increased solar absorption efficiency and efficient charge-separation and transfer of BixIn2-xO3 also contribute to the improved photocatalytic performance. These traits exemplify the opportunities that exist for atom-scale engineering in heterogeneous CO2 photocatalysis, another step towards the vision of the solar CO2 refinery.
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