[Cp*Rh(bpy)H2O]2+自组装CdIn2S4花状微球的高效光催化NADH再生与酶促CO2还原

引用本文: 高春慧, 李璐嵘, 彭官威, 沈锦妮, 戴文新, 张子重. [Cp*Rh(bpy)H₂O]²⁺自组装CdIn₂S₄花状微球的高效光催化NADH再生与酶促CO₂还原[J]. 物理化学学报, 2026, 42(3): 100165. doi: 10.1016/j.actphy.2025.100165 shu

Citation: Chunhui Gao, Lurong Li, Guanwei Peng, Jinni Shen, Wenxin Dai, Zizhong Zhang. Efficient photocatalytic NADH regeneration and enzymatic CO₂ reduction over[Cp*Rh(bpy)H₂O]²⁺ self-assembled CdIn₂S₄ flowerlike microspheres[J]. Acta Physico-Chimica Sinica, 2026, 42(3): 100165. doi: 10.1016/j.actphy.2025.100165 shu

[Cp*Rh(bpy)H₂O]²⁺自组装CdIn₂S₄花状微球的高效光催化NADH再生与酶促CO₂还原

1.
福州大学, 化工学院, 福建福州 350116;
2.
福州大学, 化学学院, 核生化防护化学全国重点实验室, 福建福州 350116;
3.
清源创新实验室, 福建泉州 362801

通讯作者: 张子重,Email:z.zhang@fzu.edu.cn

基金项目:
本研究获得国家自然科学基金(项目编号22372041)、福建省科技重大专项(编号2021YZ037005)以及核生化防护化学全国重点实验室(编号SKLNBC2023-07)资助

摘要: 将光催化辅因子再生与酶催化偶联有助于实现可持续的CO₂增值利用，但该技术仍面临氢源有限、均相介体及光生空穴诱导酶失活等挑战。本研究表明，L-抗坏血酸(L-AA)的低氧化电位可增强质子供给并促进[Cp*Rh(bpy)H]⁺中间体形成。仅需0.26 mg (≈ 0.12 mmol L^-1) [Cp*Rh(bpy)Cl]Cl即可实现高效/选择性还原型烟酰胺腺嘌呤二核苷酸(NADH)再生，其效率是典型牺牲剂三乙醇胺(TEOA)的两倍以上。本研究开发了一种将[Cp*Rh(bpy)H₂O]²⁺静电自组装在CdIn₂S₄微球光催化剂上的新策略。这种创新集成方式通过空间分区将游离介体和光生空穴与酶隔离，有效抑制了酶失活。最优集成光催化体系在420 nm光照40 min内实现90%的NADH再生效率，优于已报道的同类体系。与甲酸脱氢酶(FDH)偶联时，该集成体系甲酸生成速率达443.5 μmol g^-1 h^-1 (明暗循环)和202.7 μmol g^-1 h^-1 (持续光照)，分别是含游离介体体系的1.2倍和3.2倍。本研究为光驱动辅酶再生及酶催化CO₂合成高附加值化学品提供了高效可持续的新策略。

关键词:

English

Efficient photocatalytic NADH regeneration and enzymatic CO₂ reduction over[Cp*Rh(bpy)H₂O]²⁺ self-assembled CdIn₂S₄ flowerlike microspheres

1.
College of Chemical Engineering, Fuzhou University, Fuzhou 350116, Fujian Province, China;
2.
State Key Laboratory of Chemistry for NBC Hazards Protection, College of Chemistry, Fuzhou University, Fuzhou 350116, Fujian Province, China;
3.
Qingyuan Innovation Laboratory, Quanzhou 362801, Fujian Province, China

Corresponding author: Zizhong Zhang, z.zhang@fzu.edu.cn

Received Date: 15 July 2025
Accepted Date: 17 August 2025
Revised Date: 14 August 2025

Abstract: Integrating photocatalytic cofactor regeneration with enzymatic cascades enables sustainable CO₂ valorization but faces challenges like limited hydrogen sources and homogeneous mediator and photogenerated holes-induced enzyme deactivation. This study demonstrates that the low oxidation potential of L-ascorbic acid (L-AA) can enhance proton supply and promote the formation of[Cp*Rh(bpy)H]⁺ intermediates. Only 0.26 mg (≈ 0.12 mmol L^-1)[Cp*Rh(bpy)Cl]Cl can achieve efficient/selective reduced nicotinamide adenine dinucleotide (NADH) regeneration, which is more than twice as effective as the typical sacrificial agent triethanolamine (TEOA). A novel strategy was developed via electrostatic self-assembly of [Cp*Rh(bpy)H₂O]²⁺ onto CdIn₂S₄ microsphere photocatalysts. This innovative integration physically separated free mediators and photogenerated holes from enzymes, effectively suppressing enzyme deactivation through spatial compartmentalization. The optimal integrated photocatalytic system achieved 90% NADH regeneration efficiency within 40 min of 420 nm light irradiation, outperforming previously reported systems. When coupled with formate dehydrogenase (FDH), the integrated system achieved formic acid generation rates of 443.5 μmol g^-1 h^-1 (one light-dark cycle) and 202.7 μmol g^-1 h^-1 (continuous light), representing 1.2- and 3.2-fold improvements over free mediator systems, respectively. This study provides an efficient and sustainable new strategy for light driven coenzyme regeneration and enzyme catalyzed CO₂ synthesis of high value-added chemicals.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

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通讯作者: 张子重,Email:z.zhang@fzu.edu.cn

English

Efficient photocatalytic NADH regeneration and enzymatic CO₂ reduction over[Cp*Rh(bpy)H₂O]²⁺ self-assembled CdIn₂S₄ flowerlike microspheres

Corresponding author: Zizhong Zhang, z.zhang@fzu.edu.cn

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