2023
DOI: 10.1002/adma.202210669
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Electronic State and Microenvironment Modulation of Metal Nanoparticles Stabilized by MOFs for Boosting Electrocatalytic Nitrogen Reduction

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Cited by 83 publications
(44 citation statements)
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“…As listed in entries 1–3, the substrates with relatively smaller sizes can be efficiently catalyzed to convert into the corresponding cyclic carbonates. However, as the number of substituent atoms increases, their yield shows a slightly decreasing trend, which should be ascribed to the increased weaker interactions such as hydrogen bonds between the host framework of NUC-101a and epoxides and derived intermediates and products. , Compared to others, aromatic epoxides of SO and 2-(phenoxymethyl)­oxirane in the catalytic reaction system could display satisfied transformation, which are consistent with most of the reported MOF-canalization cycloaddition and should be due to the more convenient mass transfer between Lewis acid–base sites and substrate molecules of epoxides and CO 2 . This could be proved by the following control experiments with NUC-101a being replaced by H 5 BDTP, Dy 2 O 3 , or H 5 BDTP/Dy 2 O 3 , which caused a significant decrease in conversion rate, shown in Table S6. As for cyclohexene oxide, a much lower yield was observed.…”
Section: Resultssupporting
confidence: 81%
“…As listed in entries 1–3, the substrates with relatively smaller sizes can be efficiently catalyzed to convert into the corresponding cyclic carbonates. However, as the number of substituent atoms increases, their yield shows a slightly decreasing trend, which should be ascribed to the increased weaker interactions such as hydrogen bonds between the host framework of NUC-101a and epoxides and derived intermediates and products. , Compared to others, aromatic epoxides of SO and 2-(phenoxymethyl)­oxirane in the catalytic reaction system could display satisfied transformation, which are consistent with most of the reported MOF-canalization cycloaddition and should be due to the more convenient mass transfer between Lewis acid–base sites and substrate molecules of epoxides and CO 2 . This could be proved by the following control experiments with NUC-101a being replaced by H 5 BDTP, Dy 2 O 3 , or H 5 BDTP/Dy 2 O 3 , which caused a significant decrease in conversion rate, shown in Table S6. As for cyclohexene oxide, a much lower yield was observed.…”
Section: Resultssupporting
confidence: 81%
“…As shown in Figure S7, the value for the isosteric heat of adsorption ( Q st ) at lower coverage was estimated to be 27.5 kJ/mol, indicating that the adsorption capacity of CO 2 is mainly physical adsorption. On account of references, the host framework of NUC-110Gd has adsorption and desorption regeneration performance due to the relatively low adsorption heat. As a comparison, an as-synthesized sample of NUC-110Gd without activation was tested for the adsorption capacity of CO 2 , which displayed a very low adsorption value, shown in Figure S8.…”
Section: Resultsmentioning
confidence: 99%
“…Ammonia (NH 3 ) is an indispensable chemical in agriculture, chemical industry, refrigeration, hydrogen energy and healthcare. [1][2][3] However, the conventional Haber-Bosch process, which dominates industrial ammonia synthesis, requires high temperature and pressure, resulting in a significant environmental impact. [4][5][6] To address this issue, electrocatalytic nitrogen reduction reaction (ENRR) is being considered as an alternative approach to produce NH 3 under mild conditions, which is more sustainable and environmentally friendly.…”
Section: Introductionmentioning
confidence: 99%