高效可见光响应微生物/光电化学耦合人工光合作用系统

doi:10.11949/0438-1157.20211197

摘要/Abstract

摘要：

人工光合作用系统可以利用太阳能将二氧化碳转化为高附加值的化学产品，能够有效地解决人类面临的能源与环境问题，极具发展前景。然而，人工光合作用系统面临产物选择性差、过电位高、太阳能利用率低等重大挑战。本文提出了一种新型微生物/光电化学耦合人工光合作用系统，该系统由固碳产甲烷微生物阴极和复合光阳极组成，其中复合光阳极由TiO₂电极与硅太阳能电池串联组成。该耦合系统在仅输入太阳能且不施加外部偏压的条件下，可实现化学燃料甲烷的产生。甲烷产量高达（10.7±0.2） L·d^-1·m^-2，相比已有研究高出13倍，同时该耦合系统固碳产甲烷的法拉第效率高达98.5%±2.1%，远高于传统的人工光合作用系统。该新型人工光合作用系统的提出，为制取具有高附加值的化学产品和发展可再生能源提供了新的思路。

关键词: 人工光合作用, 复合光阳极, 生物催化, CO₂还原

Abstract:

The artificial photosynthesis system can use solar energy to convert carbon dioxide into high value-added chemical products, which can effectively solve the energy and environmental problems faced by mankind, and has great development prospects. However, artificial photosynthesis systems face major challenges such as poor product selectivity, high overpotential, and low solar energy utilization. Here we present a hybrid microbial-photoelectrochemical system comprised of a monolithic photoanode, which is assembled by attaching a silicon cell at the reverse side of a TiO₂ nanorod array for water oxidation, and a biocathode that is capable of reducing CO₂ to CH₄. The hybrid system shows an excellent CH₄ production rate of (10.7±0.2) L·d^-1·m^-2, around 13 times higher than that of previous studies, and achieved a highly selective CO₂ reduction to CH₄ with a Faradaic efficiency up to 98.5%±2.1%. This work proposes an effective approach for the generation of valuable products using artificial photosynthesis.

Key words: artificial photosynthesis, monolithic photoanode, biocatalysis, CO₂ reduction

中图分类号:

TK 621.1

王淋, 付乾, 肖帅, 李卓, 李俊, 张亮, 朱恂, 廖强. 高效可见光响应微生物/光电化学耦合人工光合作用系统[J]. 化工学报, 2022, 73(2): 887-893.

Lin WANG, Qian FU, Shuai XIAO, Zhuo LI, Jun LI, Liang ZHANG, Xun ZHU, Qiang LIAO. High-efficient visible light responsive microbial photoelectrochemical system for CO₂ reduction to CH₄[J]. CIESC Journal, 2022, 73(2): 887-893.

图/表 5

图1 微生物/光电化学耦合系统工作原理图

Fig.1 Working principle of the hybrid microbial-photoelectrochemical system

图2 复合光阳极结构图

Fig.2 Construction of the monolithic photoanode

图3 FTO上生长TiO2纳米线阵列的扫描电子显微镜图[(a) 俯视图；(b) 截面图]； TiO2纳米线阵列和硅电池的紫外可见吸收光谱(c)；在光强为100 mW·cm-2、光周期开/关的条件下TiO2纳米线阵列的线性伏安扫描曲线（扫描速率：10 mV·s-1）(d)

Fig.3 SEM images of TiO2 nanowire arrays[(a)top-view;(b)cross view]; UV-vis reflectance of TiO2 and silicon cell(c); LSV of TiO2 photoanode with light on/off cycle (scan rate:10 mV·s-1)(d)

图4 微生物启动电流(a)；微生物启动阴阳极电位(b)；微生物阴极循环伏安曲线(c)

Fig.4 Current curves started up (a); Potential curves of electrodes (b); CV analyses of biocathode and abiotic (c)

图5 耦合系统的电流（红线），复合光阳极与非生物纯碳布电极系统的电流（蓝线），TiO2光阳极与微生物阴极系统的电流（黄线）(a)；光周期开/关条件下耦合系统的电位图(b)；耦合系统连续运行30 h电流图（红线）与甲烷产量（蓝线）(c)

Fig.5 Current generation of the hybrid system (a); Potential-responses of the cathode (blue curve) and photoanode (red curve) to the light on and off (b);CH4 production and the Faradaic efficiency of the hybrid system (c)

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