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Efficient NADH Regeneration without Electron Mediator toward Enzymatic CO2 Reduction Enabled by a Lawn-like TP-COFs/Ti3C2Tx (MXene) Photocatalyst
ACS Sustainable Chemistry & Engineering ( IF 8.4 ) Pub Date : 2024-04-24 , DOI: 10.1021/acssuschemeng.3c07466
Ping Wei 1 , Jinfeng Dong 1 , Xingyue Gao 2 , Lekai Chang 2 , Zhipeng Huang 2 , Hailong Zheng 2 , Simon Ming-Yuen Lee 3 , Wen-Yong Lou 4 , Chao Peng 2, 5, 6
Affiliation  

Photocatalytic nicotinamide adenine dinucleotide (NADH) regeneration coupled with enzymatic CO2 reduction holds significance for global sustainable development. In this work, acrylonitrile-linked covalent organic frameworks (COFs) loaded on NH2–Ti3C2Tx (MXene) forms a lawn-like TP-COFs/Ti3C2Tx (TCM) photocatalyst for NADH regeneration. The optimum photocatalyst TCM-15% achieves a 95% NADH regeneration yield within 30 min. More importantly, the TCM-15% obtains 46% NADH regeneration yield without an electron mediator ([Cp*Rh(bpy)(H2O)]2+), even higher than that of the pure TP-COFs with an electron mediator (42%). In the presence and absence of an electron mediator, the NADH regeneration TOF values of TCM-15% were 3.69 and 1.42 h–1, respectively, which were 4.05 and 4.90 times higher than those of pure TP-COFs. Subsequently, in the photoenzymatic catalytic cascade system, the formate formation rates reached 2380 and 543 μmol g–1 h–1, with and without an electron mediator, respectively. This work has laid a great foundation for achieving efficient NADH regeneration and cascade enzyme catalysis without an electron mediator.

中文翻译:

草坪状 TP-COF/Ti3C2TX (MXene) 光催化剂实现酶促 CO2 还原,无需电子介体即可高效再生 NADH

光催化烟酰胺腺嘌呤二核苷酸(NADH)再生与酶促CO 2还原对全球可持续发展具有重要意义。在这项工作中,负载在NH 2 –Ti 3 C 2 T x (MXene)上的丙烯腈连接的共价有机框架(COF)形成了草坪状的TP-COFs/Ti 3 C 2 T x (TCM)光催化剂,用于NADH再生。最佳光催化剂TCM-15%可在30分钟内实现95%的NADH再生率。更重要的是,TCM-15%在没有电子介体的情况下获得了46%的NADH再生率([Cp*Rh(bpy)(H 2 O)] 2+),甚至高于有电子介体的纯TP-COFs (42%)。在电子介体存在和不存在的情况下,TCM-15%的NADH再生TOF值分别​​为3.69和1.42 h –1,分别是纯TP-COFs的4.05和4.90倍。随后,在光酶催化级联系统中,有或没有电子介体时,甲酸形成率分别达到 2380 和 543 μmol g –1 h –1 。该工作为实现无电子介体的NADH高效再生和级联酶催化奠定了良好的基础。
更新日期:2024-04-24
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