journal article·2024-05-01

Cu–phen Coordination Enabled Selective Electrocatalytic Reduction of CO2 to Methane

Haiyan Hu, Shiting Qian, Qin Shi, Minxing Du, Ning Sun, Yong Ding, Jun Li, Qiquan Luo, Zhen Li, Lin He, Yuxia Sun, Yuehui Li

ACS Applied Materials & Interfaces· Volume 16· Issue 17
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Abstract

Manipulation of selectivity in the catalytic electrochemical carbon dioxide reduction reaction (eCO 2 RR) poses significant challenges due to inevitable structure reconstruction. One approach is to develop effective strategies for controlling reaction pathways to gain a deeper understanding of mechanisms in robust CO 2 RR systems. In this work, by precise introduction of 1,10-phenanthroline as a bidentate ligand modulator, the electronic property of the copper site was effectively regulated, thereby directing selectivity switch. By modification of [Cu 3 (btec)(OH) 2 ] n, the use of [Cu 2 (btec)(phen) 2 ] n ·(H 2 O) n achieved the selectivity switch from ethylene (faradaic efficiency (FE) = 41%, FE C2+ = 67%) to methane (FE CH 4 = 69%). Various in situ spectroscopic characterizations revealed that [Cu 2 (btec)(phen) 2 ] n ·(H 2 O) n promoted the hydrogenation of *CO intermediates, leading to methane generation instead of dimerization to form C 2+ products. Acting as a delocalized π-conjugation scaffold, 1,10-phenanthroline in [Cu 2 (btec)(phen) 2 ] n ·(H 2 O) n helps stabilize Cu δ+ . This work presents a novel approach to regulate the coordination environment of active sites with the aim of selectively modulating the CO 2 RR.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: CO2 Reduction Techniques and Catalysts · Ionic liquids properties and applications · Carbon dioxide utilization in catalysis

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization; State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics (LICP), Chinese Academy of Sciences, Lanzhou 730000, P. R. China

State Key Laboratory of Applied Organic Chemistry, Key Laboratory of Advanced Catalysis of Gansu Province, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, P. R. China

University of Chinese Academy of Sciences, Beijing 100049, P. R. China

School of Chemistry and Chemical Engineering, School of Materials Science and Engineering, Institute of Physical Science and Information Technology, Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized Materials, Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education, Anhui University, Hefei 230601, Anhui P. R. China

Frontiers Science Center for Transformative Molecules, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai 200240, P. R. China

Funding

Natural Science Foundation of Jiangsu Province · National Natural Science Foundation of China

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