分子催化剂电化学活化氮气用于可持续合成氨
Molecular Catalysts for Electrochemical Nitrogen Activation toward Sustainable Ammonia Synthesis
分子催化剂电化学活化氮气用于可持续合成氨 |
| 韩金秀, 薛皓, 付先彪 |
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Molecular Catalysts for Electrochemical Nitrogen Activation toward Sustainable Ammonia Synthesis |
| Jin-Xiu Han, Hao Xue, Xian-Biao Fu |
| Fig. 14. (a) CVs of the catholyte under standard PNPMoBr3 electrocatalytic conditions after 0.1-1.3 C of charge has passed; inset: NH3 production plotted as a function of charge. (b) CVs of SmI3 (2 mmol·L-1, blue), PNPMoBr3 (0.5 mmol·L-1, pink), and PNPMo(N)I (0.5 mmol·L-1, red). (c) CVs of PNPMo(N)I (0.46 mmol·L-1) with LutHNTf2 (80 equiv., blue) under N2, overlaid with the LutHNTf2 background; inset: evolution of the MoV/IV couple upon sequential addition of LutHNTf2 (blue) and Lut (4-160 equiv; light blue to red). (d) Proposed electron-delivery pathways for the 1 H+/1 e− step converting PNPMo(N)I toward NH3. Direct reduction of the MoV/IV couple requires Eapp < −1.6 V vs. Fc+/0, where competing LutH+ reduction lowers FE. With Sm, the SmIII/II mediator delivers electrons to the MoV/IV couple around −1.45 V vs. Fc+/0, accelerating a limiting ET step while suppressing background acid reduction. Reproduced with permission of Ref. [ |
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