2023
DOI: 10.1021/acs.accounts.2c00832
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Structure–Reactivity Relationships in Borane-Based FLP-Catalyzed Hydrogenations, Dehydrogenations, and Cycloisomerizations

Abstract: Conspectus The activation of molecular hydrogen by main-group element catalysts is an extremely important approach to metal-free hydrogenations. These so-called frustrated Lewis pairs advanced within a short period of time to become an alternative to transition metal catalysis. However, deep understanding of the structure–reactivity relationship is far less developed compared to that of transition metal complexes, although it is paramount for advancing frustrated Lewis pair chemistry. In this Account, we provi… Show more

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Cited by 17 publications
(7 citation statements)
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“…In the discharge process, the Li─In bonds gradually become stronger, transforming into a borane structure of the same group. [ 35 ] The crystal structure of Li 3 N is also shown in Figure S15 (Supporting Information). In the charge process, the In atoms rebuild the bonds and the Li atoms redistribute in the cell.…”
Section: Resultsmentioning
confidence: 99%
“…In the discharge process, the Li─In bonds gradually become stronger, transforming into a borane structure of the same group. [ 35 ] The crystal structure of Li 3 N is also shown in Figure S15 (Supporting Information). In the charge process, the In atoms rebuild the bonds and the Li atoms redistribute in the cell.…”
Section: Resultsmentioning
confidence: 99%
“…Main-group element catalysts are desirable alternatives to transition-metal catalysts because of their natural abundance and low cost. , More importantly, main-group element catalysts have low binding affinity to CO, owing to the lack of suitable π-back-bonding orbitals . This implies good tolerance to CO and inspires us to explore main-group element catalysts for the indirect hydrogenation of CO to methanol.…”
Section: Introductionmentioning
confidence: 99%
“…These remarkable bifunctional metal catalysts facilitate indirect CO hydrogenation but are still limited by high reaction temperatures and low yields, which could be associated with the deactivation of transition-metal catalysts in the presence of CO. 32 Main-group element catalysts are desirable alternatives to transition-metal catalysts because of their natural abundance and low cost. 33,34 More importantly, main-group element catalysts have low binding affinity to CO, owing to the lack of suitable π-back-bonding orbitals. 35 This implies good tolerance to CO and inspires us to explore main-group element catalysts for the indirect hydrogenation of CO to methanol.…”
Section: Introductionmentioning
confidence: 99%
“…Recent advancements in cheminformaticsbased machine learning (ML) offer chemists a way to bypass traditional Edisonian empiricism and develop more efficient approaches to optimizing catalysts 1-4 . Several groups have reported successful demonstrations of ML-driven optimizations of homogeneous catalysts such as phosphoric acids and Lewis-basic ligands for metal-based catalysts involving phosphines, N-heterocyclic carbenes, and nitrogen-based ligands [5][6][7][8][9][10][11][12][13][14][15][16][17][18] .Recent progress in frustrated Lewis pairs (FLPs) 19,20 has expanded the practical and sustainable application of main-group catalysis, e.g., enabling the hydrogenation of unsaturated molecules without toxic/ precious metals [21][22][23][24][25][26] . In this context, the main-group-catalyzed reductive alkylation of amines with carbonyl compounds and H 2 via the generation of FLP species has been widely accepted as a wasteminimizing process that generates valuable N-alkylated amines, whereby H 2 O is the only by-product 23,[27][28][29][30][31] .…”
mentioning
confidence: 99%
“…Recent progress in frustrated Lewis pairs (FLPs) 19,20 has expanded the practical and sustainable application of main-group catalysis, e.g., enabling the hydrogenation of unsaturated molecules without toxic/ precious metals [21][22][23][24][25][26] . In this context, the main-group-catalyzed reductive alkylation of amines with carbonyl compounds and H 2 via the generation of FLP species has been widely accepted as a wasteminimizing process that generates valuable N-alkylated amines, whereby H 2 O is the only by-product 23,[27][28][29][30][31] .…”
mentioning
confidence: 99%