利用光驱动的生物杂合系统实现CO2转化生产化学品

doi:10.1016/S1872-2067(23)64643-1

催化学报 ›› 2024, Vol. 60: 294-303.DOI: 10.1016/S1872-2067(23)64643-1

利用光驱动的生物杂合系统实现CO₂转化生产化学品

干雅梅^a, 柴甜甜^a, 张健^a, 高聪^a, 宋伟^b, 吴静^b, 刘立明^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:2024-01-07 接受日期:2024-02-28 出版日期:2024-05-18 发布日期:2024-05-22
通讯作者: *电子信箱: xlchen@jiangnan.edu.cn (陈修来).
基金资助:
国家自然科学基金项目(22122806);国家自然科学基金项目(22038005);江苏省自然科学基金项目(BK20211529);江苏省自然科学基金项目(BK20220022);中央高校基本科研业务费专项资金项目(JUSRP622001);中央高校基本科研业务费专项资金项目(JUSRP622011);国家双一流轻工技术经费项目(QGJC20230101)

Light-driven CO₂ utilization for chemical production in bacterium biohybrids

Yamei Gan^a, Tiantian Chai^a, Jian Zhang^a, Cong Gao^a, Wei Song^b, Jing Wu^b, Liming Liu^a, Xiulai Chen^a^,^*()

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

Received:2024-01-07 Accepted:2024-02-28 Online:2024-05-18 Published:2024-05-22
Contact: *E-mail: xlchen@jiangnan.edu.cn (X. Chen).
Supported by:
National Natural Science Foundation of China(22122806);National Natural Science Foundation of China(22038005);Provincial Natural Science Foundation of Jiangsu Province(BK20211529);Provincial Natural Science Foundation of Jiangsu Province(BK20220022);Fundamental Research Funds for the Central Universities(JUSRP622001);Fundamental Research Funds for the Central Universities(JUSRP622011);National First-class Discipline Program of Light Industry Technology and Engineering(QGJC20230101)

摘要/Abstract

摘要：

太阳能作为清洁能源之一, 为缓解化石燃料枯竭和温室气体排放等问题提供了一种高效、经济、可持续的解决方案. 自然界中的植物和光合微生物通过自身的光合系统收集并转化太阳能, 从而生产生物燃料和生物化学品. 然而, 由于自然光合系统存在光吸收范围相对较窄、光生电子在传输过程中易损耗等问题, 限制了太阳能到化学品的转化效率. 为了解决上述难题, 科研人员模仿自然光合作用中的关键部分, 探索构建人工光合系统, 相关研究引起了广泛关注.

本文通过将碲化镉量子点(CdTe QDs)与大肠杆菌(E. coli)相耦合, 构建了一种光驱动无机-生物杂合系统(IBPHS), 用于捕获太阳能并驱动CO₂转化合成高价值化学品. 该系统主要由光催化模块和生物催化模块组成. 在光催化模块中, 通过生物合成CdTe QDs进行光能捕获, 并将其转化为电子. 通过敲除E. coli的Cd²⁺外排蛋白(ZNTA)编码基因, 实现了E. coli胞内Cd²⁺过量积累. 通过“时空耦合”方式, 并借助共聚焦显微镜、高分辨率透射电镜和X射线能谱分析, 确认了CdTe QDs在E. coli胞内的组装合成. 利用紫外-可见分光光度计研究了光催化模块对光子的吸收能力. 结果表明, 光催化模块的吸收峰位于400‒420 nm. 利用瞬时光电流, 评估了光催化模块的光生电子能力. 实验发现, 该模块可以产生0.07 μA光电流, 表明完成了光催化模块的构建. 在生物催化模块中, 将光催化模块产生的电子用于还原NAD⁺再生NADH. 采用NADH生物传感器, 分析了E. coli胞内NADH含量, 结果表明, 在蓝光照射下E. coli胞内NADH含量比黑暗条件下提高了5.1倍. 在此基础上, 通过表达NADH依赖型乳酸脱氢酶(LDH)将丙酮酸还原为乳酸, 在蓝光光照下乳酸积累量达到了0.44 g/L, 而黑暗条件下无乳酸积累, 从而验证了生物催化模块的有效性. 基于光催化模块和生物催化模块, 进一步组装构建了IBPSH, 用于驱动CO₂还原合成甲酸和丙酮酸. 在蓝光照射下, IBPHS能够合成0.65 g/L甲酸和0.18 g/L丙酮酸, 其CO₂利用速率分别达到51.98 mg/gDCW/h和21.92 mg/gDCW/h, 超过了光合细菌.

综上所述, 本文利用光催化模块与生物催化模块相耦合的方式, 组装构建了一种新型的人工光合系统, 实现了光驱动CO₂还原合成高附加值化学品, 为理性设计材料-生物杂合系统提供了借鉴, 同时也为挖掘绿色生物制造潜力、开发太阳能化学制造平台提供参考.

关键词: 人工光合系统, CO₂利用, 光能转换, CdTe生物合成, NADH再生

Abstract:

Artificial photosynthetic systems provide an alternative approach for the sustainable, efficient, and versatile production of biofuels and biochemicals. However, improving the efficiency of electron transfer between semiconductor materials and microbial cells remains a challenge. In this study, an inorganic-biological photosynthetic biohybrid system (IBPHS) consisting of photocatalytic and biocatalytic modules was developed by integrating cadmium telluride quantum dots (CdTe QDs) with Escherichia coli cells. A photocatalytic module was constructed by biosynthesizing CdTe QDs to capture light and generate electrons. The biocatalytic module was built by converting photo-induced electrons to enhance NADH regeneration; thus, the NADH content in E. coli under blue light increased by 5.1-fold compared to that in darkness. Finally, IBPHS was utilized to drive CO₂ reduction pathways for versatile bioproduction such as formate and pyruvate, with CO₂ utilization rates up to 51.98 and 21.92 mg/gDCW/h, respectively, exceeding that of cyanobacteria. This study offers a promising platform for the rational design of biohybrids for efficient biomanufacturing processes with high complexity and functionality.

Key words: Artificial photosynthetic system, CO₂ utilization, Solar energy conversion, CdTe biosynthesis, NADH regeneration

干雅梅, 柴甜甜, 张健, 高聪, 宋伟, 吴静, 刘立明, 陈修来. 利用光驱动的生物杂合系统实现CO₂转化生产化学品[J]. 催化学报, 2024, 60: 294-303.

Yamei Gan, Tiantian Chai, Jian Zhang, Cong Gao, Wei Song, Jing Wu, Liming Liu, Xiulai Chen. Light-driven CO₂ utilization for chemical production in bacterium biohybrids[J]. Chinese Journal of Catalysis, 2024, 60: 294-303.

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Fig. 1. Designing inorganic-biological photosynthetic biohybrid system (IBPHS) for CO2 utilization. IBPHS consisted of the photocatalytic and biocatalytic modules. The photocatalytic module was constructed by biosynthesizing CdTe QDs to capture light and then generate electrons. The biocatalytic module was built by converting photo-induced electrons to enhance NADH regeneration. IBPHS was utilized to drive CO2 reduction pathways for versatile bioproduction such as formate and pyruvate. VB: valence band; CB: conduction band; e?: electron; CO2: carbon dioxide; HWLS: half-Wood-Ljungdahl-formolase.

Fig. 2. Constructing inorganic-biological photosynthetic biohybrid system (IBPHS). (a) ICP-MS showing the absorption of Cd2+ ions. (b?d) CLSM image showing the biosynthesis of CdTe nanoparticles in E. coli JZ. (e) Cross-section TEM image showing the localization of CdTe nanoparticles in E. coli cells. The black dots represent CdTe nanoparticles. HAADF-STEM images (f?i) and EDS mapping (j) of CdTe nanoparticles. (k) XPS analysis of CdTe nanoparticles. (l) HETEM image and lattice fringes of CdTe nanoparticles.

Fig. 3. Evaluating inorganic-biological photosynthetic biohybrid system (IBPHS). (a) UV-vis diffuse reflectance spectra of E. coli strains. (b) Bandgap width of CdTe QDs. (c) Transient photocurrent of IBPHS. (d) Electrochemical impedance spectroscopy of IBPHS. (e,f) Intracellular NADH contents of IBPHS. (g,h) Evaluation of the regenerated NADH for bioproduction in vivo and in vitro, respectively.

Fig. 4. Converting CO2 to formate by the inorganic-biological photosynthetic biohybrid system (IBPHS). (a) Photocatalytic reduction of CO2 for formate production in vitro. (b) Photocatalytic reduction of CO2 for formate production in vivo. (c) Optimizing FDH expression by coupling the ribosome-binding site with plasmids. (d) Formate production by optimizing FDH expression.

Fig. 5. Converting CO2 to pyruvate by the inorganic-biological photosynthetic biohybrid system (IBPHS). (a) Photocatalytic reduction of CO2 for pyruvate production in vivo. (b) Engineered E. coli strains for pyruvate production. (c) Pyruvate production with E. coli FH under light and dark conditions. (d) CO2-fixing rate of E. coli FH under light and dark conditions. pyk: pyruvate kinase; Fhs: formyl-tetrahydrofolate cyclohydrolase; FchA: methylene-THF dehydrogenase; FolD: methylene-THF reductase; FLS: formolase; DHAK: dihydroxyacetone kinase.

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利用光驱动的生物杂合系统实现CO₂转化生产化学品

Light-driven CO₂ utilization for chemical production in bacterium biohybrids

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