分子科学学报2024,Vol.40Issue(5) :411-420.DOI:10.13563/j.cnki.jmolsci.2024.05.104

受天然叶绿体启发构建具有高效电荷转移机制的Z型异质结以促进光催化二氧化碳还原

Inspired by natural chloroplasts to construct Z-scheme heterojunction with efficient charge transfer mechanism for boosting photocatalytic carbon dioxide reduction

柳子璇 周想 宋婷婷 姚瑞琪 赵钊 郎中玲 李英奇 谭华桥 王永慧 李阳光
分子科学学报2024,Vol.40Issue(5) :411-420.DOI:10.13563/j.cnki.jmolsci.2024.05.104

受天然叶绿体启发构建具有高效电荷转移机制的Z型异质结以促进光催化二氧化碳还原

Inspired by natural chloroplasts to construct Z-scheme heterojunction with efficient charge transfer mechanism for boosting photocatalytic carbon dioxide reduction

柳子璇 1周想 1宋婷婷 1姚瑞琪 1赵钊 1郎中玲 1李英奇 1谭华桥 1王永慧 1李阳光1
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作者信息

  • 1. 东北师范大学化学学院,多酸与网格材料化学教育部重点实验室,吉林长春 130024
  • 折叠

摘要

为了缓解碳基燃料带来的日益严重的生态威胁,通过模拟光合作用机制来构建Z型异质结提供了一种有前景的方法,以实现太阳能驱动的二氧化碳还原为高附加值化学燃料.本文设计并制备了一种基于静电相互作用将类金属卟啉Cox-CN与Keggin型POM(PMo10V2O40 5-)偶联的Z机制复合光催化剂.由于其氧化还原性质和电荷转移机制与绿色植物中的叶绿素P700和P680相似,复合异质结表现出宽光谱吸收能力和强CO2吸收能力,并抑制了光生载流子的复合.在可见光照射下,最佳的0.05PMo10V2/Co1-CN异质结显示出最高的CO产量,为101.38μmol·g-1·h-1,分别比CN和Co1-CN增加了约250倍和约9倍,同时抑制了竞争性H2的产生.这项工作为开发高效、低成本的Z机制CO2转化光催化剂提供了一种有效的设计策略.

Abstract

To alleviate the growing serious ecological threats brought by carbon-based fuels,it is a promis-ing approach to construct a Z-scheme heterojunction via simulating the photosynthetic mechanism for so-lar-driven CO2 reduction into high value-added chemical fuels.Herein,we design and prepare a Z-scheme composite photocatalyst based on coupling metalloporphyrin-like Cox-CN with Keggin-type POMs(PMo10 V2 O405-)by electrostatic interactions.By virtue of the redox property and charge transfer mecha-nism similar to chlorophyll P700 and P680 in green plants,the composite heterojunction exhibits broad-spectrum absorption and strong CO2 absorption capacity,as well as the inhibition of the recombination of photo-introduced carriers.Under visible light irradiation,the optimized 0.05PMo10V2/Co1-CN heterojunc-tion shows the highest CO yield of 101.38 μmol·g-1·h-1,which is increased by about 250 and 9 times compared with those of CN and Co1-CN,respectively,and concomitantly inhibits competitive H2 genera-tion.This work provides a promising strategy to develop high-efficiency and low-cost Z-scheme photocata-lysts for CO2 conversion.

关键词

仿生Z型异质结/多金属氧酸盐/类金属卟啉钴-碳氮纳米片/静电自组装/光催化CO2还原

Key words

biomimetic Z-scheme heterojunction/polyoxometalates/metalloporphyrin-like Co-CN nanoshe-ets/electrostatic self-assembly/photocatalytic CO2 reduction

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出版年

2024
分子科学学报
中国化学会

分子科学学报

CSTPCD
影响因子:0.434
ISSN:1000-9035
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