二氧化碳电化学还原
多金属氧酸盐
一氧化碳
卟啉
催化作用
化学
金属有机骨架
光催化
星团(航天器)
光化学
二氧化碳
碳纤维
金属
无机化学
甲烷
氧化还原
材料科学
有机化学
复合数
吸附
程序设计语言
复合材料
计算机科学
作者
Qing Huang,Qian Niu,Xiufen Li,Jiang Liu,Shengnan Sun,Long‐Zhang Dong,Shun-Li Li,Yue-Peng Cai,Ya‐Qian Lan
出处
期刊:Science Advances
[American Association for the Advancement of Science (AAAS)]
日期:2022-12-09
卷期号:8 (49)
被引量:49
标识
DOI:10.1126/sciadv.add5598
摘要
Photo- or electroreduction of carbon dioxide into highly valued products offers a promising strategy to achieve carbon neutrality. Here, a series of polyoxometalate-based metal-organic frameworks (M-POMOFs) were constructed by metalloporphyrins [tetrakis(4-carboxyphenyl)-porphyrin-M (M-TCPPs)] and reductive POM for photo- and electrocatalytic carbon dioxide reductions (PCR and ECR, respectively), and the mysteries between the roles of single metal site and cluster in catalysis were disclosed. Iron-POMOF exhibited an excellent selectivity (97.2%) with high methane production of 922 micromoles per gram in PCR, together with superior Faradaic efficiency for carbon dioxide to carbon monoxide (92.1%) in ECR. The underlying mechanisms were further clarified. Photogenerated electrons transferred from iron-TCPP to the POM cluster for methane generation under irradiation, while the abundant electrons flowed to the center of iron-TCPP for carbon monoxide formation under the applied electric field. The specific multielectron products generated on iron-POMOF through switching driving forces to control electron flow direction between single metal site and cluster catalysis.
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