journal article·2021-03-23

Selective Etching Quaternary MAX Phase toward Single Atom Copper Immobilized MXene (Ti3C2Clx) for Efficient CO2 Electroreduction to Methanol

Qi Zhao, Chao Zhang, Riming Hu, Zhiguo Du, Jianan Gu, Yanglansen Cui, Xiao Chen, Wenjie Xu, Zongju Cheng, Songmei Li, Bin Li, Yuefeng Liu, Weihua Chen, Chuntai Liu, Jiaxiang Shang, Li Song, Shubin Yang

ACS Nano· Volume 15· Issue 3
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Abstract

Single atom catalysts possess attractive electrocatalytic activities for various chemical reactions owing to their favorable geometric and electronic structures compared to the bulk counterparts. Herein, we demonstrate an efficient approach to producing single atom copper immobilized MXene for electrocatalytic CO2 reduction to methanol via selective etching of hybrid A layers (Al and Cu) in quaternary MAX phases (Ti3(Al1-xCux)C2) due to the different saturated vapor pressures of Al- and Cu-containing products. After selective etching of Al in the hybrid A layers, Cu atoms are well-preserved and simultaneously immobilized onto the resultant MXene with dominant surface functional group (Clx) on the outmost Ti layers (denoted as Ti3C2Clx) via Cu-O bonds. Consequently, the as-prepared single atom Cu catalyst exhibits a high Faradaic efficiency value of 59.1% to produce CH3OH and shows good electrocatalytic stability. On the basis of synchrotron-based X-ray absorption spectroscopy analysis and density functional theory calculations, the single atom Cu with unsaturated electronic structure (Cuδ+, 0 < δ < 2) delivers a low energy barrier for the rate-determining step (conversion of HCOOH* to absorbed CHO* intermediate), which is responsible for the efficient electrocatalytic CO2 reduction to CH3OH.
Source: europepmc · Quality: candidate unverified · Source record ↗

Research context

OpenAlex topics: MXene and MAX Phase Materials · Advanced Photocatalysis Techniques · CO2 Reduction Techniques and Catalysts

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

Affiliations

Key Laboratory of Aerospace Advanced Materials and Performance of Ministry of Education, School of Materials Science & Engineering, Beihang University, Beijing 100191, China

Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China

National Synchrotron Radiation Laboratory, Hefei National Laboratory for Physical Sciences at the Microscale, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei, Anhui 230029, China

Dalian National Laboratory for Clean Energy (DNL), Dalian Institute of Chemical Physics, Chinese Academy of Science, 457 Zhongshan Road, 116023 Dalian, China

Key Laboratory of Materials Forming and Mold Technology (Ministry of Education), Zhengzhou University, Zhengzhou 450002, China

Funding

Natural Science Foundation of Beijing Municipality · China Postdoctoral Science Foundation · National Natural Science Foundation of China · National Postdoctoral Program for Innovative

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