光驱动一碳化合物生物转化实现节能生产化学品

doi:10.1016/S1872-2067(25)64905-9

催化学报 ›› 2026, Vol. 83: 198-208.DOI: 10.1016/S1872-2067(25)64905-9

光驱动一碳化合物生物转化实现节能生产化学品

张健^a^,¹, 干雅梅^a^,¹, 朱攀^b^,¹, 赵子涵^a, 陈修来^a^,^*()

^a江南大学生物工程学院, 工业生物技术教育部重点实验室, 江苏无锡 214122
^b江南大学生命科学与健康工程学院, 江苏无锡 214122

收稿日期:2025-08-05 接受日期:2025-09-26 出版日期:2026-04-18 发布日期:2026-03-04
通讯作者: * 电子邮箱: xlchen@jiangnan.edu.cn (陈修来).
作者简介:¹共同第一作者.
基金资助:
江苏省自然科学基金(BK20241629);江苏省合成生物基础研究中心基础研究计划(BK20233003);中央高校基本科研业务费专项资金(JUSRP124023);江苏省研究生科研与实践创新计划(KYCX24_2583)

Light-driven conversion of one-carbon compounds to achieve energy-efficient production of chemicals

Jian Zhang^a^,¹, Yamei Gan^a^,¹, Pan Zhu^b^,¹, Zihan Zhao^a, Xiulai Chen^a^,^*()

^aKey Laboratory of Industrial Biotechnology of Ministry of Education, School of Biotechnology, Jiangnan University, Wuxi 214122, Jiangsu, China
^bSchool of Life Sciences and Health Engineering, Jiangnan University, Wuxi 214122, Jiangsu, China

Received:2025-08-05 Accepted:2025-09-26 Online:2026-04-18 Published:2026-03-04
Contact: * E-mail: xlchen@jiangnan.edu.cn (X. Chen).
About author:¹Contributed equally to this work.
Supported by:
Natural Science Foundation of Jiangsu Province(BK20241629);Basic Research Program of Jiangsu Basic Research Center for Synthetic Biology(BK20233003);Fundamental Research Funds for the Central Universities(JUSRP124023);Postgraduate Research & Practice Innovation Program of Jiangsu Province(KYCX24_2583)

摘要/Abstract

摘要：

社会与工业的快速发展导致温室气体排放急剧增加, 从而加剧了气候变化和极端天气等全球性问题. 基于一碳(C1)化合物的生物制造提供了一条绿色可持续的途径, 可将二氧化碳(CO₂)等C1化合物转化为生物燃料和生物化学品. 然而, 由于天然C1化合物利用途径效率较低, 且能量与还原力供应不足, 导致当前C1生物制造的效率仍面临挑战. 为了解决上述问题, 人工光合系统通过模拟自然界的光合作用, 可以实现光驱动C1化合物的生物转化, 近年来受到了广泛的关注.
本文通过将硒化镉量子点(CdSe QDs)与大肠杆菌(E. coli)相耦合, 构建了一种光驱动的生物杂合系统(LDBS), 旨在实现高效生物转化C1化合物节能生产化学品. LDBS主要由还原力再生模块和C1固定模块组成. 在还原力再生模块中, 通过在E. coli胞内合成CdSe QDs进行光能捕获, 并将其转化为电子. 首先, 改造了E. coli底盘菌株. 通过敲除E. coli的Cd²⁺外排蛋白(ZNTA)编码基因, 实现了Cd²⁺在E. coli胞内的过量积累. 接着, E. coli胞内合成了CdSe QDs. 采用“时空耦合”的方式在E. coli中合成CdSe QDs, 并通过共聚焦显微镜、高分辨率透射电镜和X-射线能谱分析等手段验证了E. coli胞内合成的CdSe QDs. 然后, 评估了E. coli胞内自组装CdSe QDs的光电转化特性. 通过紫外-可见分光光度计研究了还原力再生模块对光子的吸收能力, 发现该模块在400‒420 nm处具有吸收峰. 利用瞬时光电流分析了还原力再生模块的光生电子能力, 发现该模块可产生0.03 μA的光电流. 通过分析胞内NADH含量, 评估了还原力再生模块用于还原NAD⁺再生NADH的能力, 结果显示, 与无CdSe QDs合成的对照组相比, E. coli胞内NADH含量提高了148.1%. 在此基础上, 通过体内和体外耦合还原力再生模块与NADH依赖型乳酸脱氢酶, 在光照条件下乳酸积累量分别提高了156.9%和193.7%, 从而进一步验证了还原力再生模块的有效性. 在C1固定模块中, 借助人工生物固碳路径, 即丝氨酸醛缩酶/苹果酸酶(SM)循环, 将C1化合物转化为乙酰辅酶A. 基于还原力再生模块和C1固定模块, 进一步组装构建了LDBS, 用于驱动C1化合物生物转化合成C2, C3和C4化合物. 采用“即插即用”的方式, 组装LDBS与SM循环及其拓展途径, 在光照条件下, LDBS能够合成1.2 mmol/L乙酰辅酶A, 284.7 μmol/L丙酮酸和385.2 μmol/L琥珀酸, C1化合物利用速率接近了蓝藻和微藻.
综上, 本文构建了一种光驱动生物杂合系统, 通过整合还原力再生模块与C1化合物固定模块, 实现了光驱动C1化合物生物转化合成多碳化学品. 该策略为未来利用C1化合物进行光驱动生物燃料与生化制品生产提供了新型平台.

关键词: CO₂固定, 生物杂合系统, CdSe, 太阳能, NADH再生

Abstract:

Societal and industrial development has caused a drastic increase in greenhouse gas emissions, leading to serious environmental problems. One-carbon (C1) based biomanufacturing offers a green and sustainable approach for converting C1 compounds such as carbon dioxide (CO₂) to biofuels and biochemicals. However, the efficiency of C1-based biomanufacturing is still challenging, due to the intrinsic inefficiency of C1-utilizing pathways and the inadequate supply of energy and reducing power. Here, a light-driven biohybrid system (LDBS) was developed to facilitate energy-efficient bioproduction by integrating reducing power regeneration and synthetic C1 fixation modules in E. coli. Reducing power regeneration module was constructed by biosynthesizing photosensitive cadmium selenide quantum dots in E. coli to enable the conversion of solar energy to reducing power, leading to a 148.1% increase in intracellular NADH contents. C1 fixation module was built by employing a new-to-nature serine aldolase/malic enzyme cycle. By integrating two modules, LDBS was programmed in a plug-and-play manner for the biosynthesis of C2, C3 and C4-compounds with C1 utilization rates approaching those of cyanobacteria and microalgae. The study demonstrates a carbon-negative platform that extends the operational scope of photobiosynthesis technologies, potentially advancing C1-based biomanufacturing for sustainability.

Key words: CO₂ fixation, Biohybrid system, CdSe, Solar energy, NADH regeneration

张健, 干雅梅, 朱攀, 赵子涵, 陈修来. 光驱动一碳化合物生物转化实现节能生产化学品[J]. 催化学报, 2026, 83: 198-208.

Jian Zhang, Yamei Gan, Pan Zhu, Zihan Zhao, Xiulai Chen. Light-driven conversion of one-carbon compounds to achieve energy-efficient production of chemicals[J]. Chinese Journal of Catalysis, 2026, 83: 198-208.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(25)64905-9

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图/表 5

Fig. 1. Designing LDBS for C1 utilization. LDBS consisted of reducing power regeneration and C1 fixation modules. Reducing power regeneration module was constructed by biosynthesizing CdSe QDs to enable the conversion of solar energy to reducing power. C1 fixation module was built by installing new-to-nature C1-fixing pathways for C1 utilization in E. coli. By coupling reducing power regeneration and C1 fixation modules, LDBS could be designed to capture solar energy for regenerating reducing power, and then reducing power could be utilized to drive the conversion of C1 compounds for bioproduction. e?: electron; Dred: reduced electron donor; Dox: oxidized electron donor; hν: incident photon; ETC: electron transport chain.

Fig. 2. Constructing reducing power regeneration module. (a) CLSM image illustrating the biosynthesis of CdSe nanoparticles in E. coli. (b) Cross-section TEM image illustrating the localization of CdSe nanoparticles in E. coli cells. c, HETEM image and lattice fringes of CdSe nanoparticles. (d?g) HAADF-STEM image of CdSe. (h?j) The mapping of EDS in E. coli JZ-CdSe. (k) ICP-MS illustrating the absorption of Cd2+ and SeO32? ions. (l) The spot scan of EDS in E. coli JZ-CdSe. (m) XPS analysis of CdSe nanoparticles. (n) Survival rate of E. coli JZ-CdSe cells.

Fig. 3. Evaluating reducing power regeneration module. (a) UV-vis DRS spectra of E. coli JZ-CdSe. (b) Bandgap width of CdSe QDs. (c) Transient photocurrent of E. coli JZ-CdSe. (d) Electrochemical impedance spectroscopy of E. coli JZ-CdSe. (e,f) The intracellular NADH contents of E. coli JZ-CdSe. (g) The absorbance of E. coli JZ-CdSe using electron acceptor methyl orange. (h) Evaluating the regenerated NADH for bioproduction in vivo. (i) Evaluating NADH regeneration for bioproduction in vitro.

Fig. 4. Developing LDBS by integrating the SM cycle and reducing power regeneration module. (a,b) LDBS was developed by assembling the SM cycle and reducing power regeneration module in vitro and in vivo. (c) Acetyl-CoA production with LDBS under light condition in vitro. (d) Acetyl-CoA production with LDBS in E. coli JZ-C2-CdSe under light condition in vivo. Sal, serine aldolase; Sda, serine deaminase; Me, malic enzyme; Mtk, malate thiokinase; Mcl, malyl-CoA lyase; Agt, aspartate-glyoxylate transaminase; e?, electron; Dred, reduced electron donor; Dox, oxidized electron donor; hν, incident photon, ETC, electron transport chain.

Fig. 5. Programming LDBS for C3-compounds and C4-compounds production. (a) The SM cycle in LDBS was extended for transforming acetyl-CoA into pyruvate by assembling SMP pathway and reducing power regeneration module. (b) Pyruvate production with E. coli JZ-C3-CdSe under light condition in vivo. (c) The SM cycle in LDBS was extended for transforming acetyl-CoA into C4-compounds by assembling SMAPS pathway and reducing power regeneration module. (d) Succinate production with E. coli JZ-C4-CdSe under light condition in vivo. Adh, acetaldehyde dehydrogenase; Pdc, pyruvate decarboxylase; Acc, acetyl-CoA carboxylase; Mcr, malonyl-CoA reductase; Pcs, multifunctional propionyl-CoA synthetase; Pcc, propionyl-CoA carboxylase; Epi, methylmalonyl-CoA epimerase; Mcm, methylmalonyl-CoA mutase; Smt, succinyl-CoA: L-malate CoA-transferase; e-, electron; Dred, reduced electron donor; Dox, oxidized electron donor; hν, incident photon, ETC, electron transport chain.

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光驱动一碳化合物生物转化实现节能生产化学品

Light-driven conversion of one-carbon compounds to achieve energy-efficient production of chemicals

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