Caizhen Yue, Xiaobo Yang, Xiong Zhang, Shifu Wang, Wei Xu, Ruru Chen, Jiuyi Wang, Jie Yin, Yanqiang Huang, Xuning Li
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引用次数: 0
Abstract
The regulation of the local microenvironment in the single‐atom catalysts affords a scheme for accelerating the overall reaction kinetics of electrochemical CO2 reduction reaction (CO2RR), which is of vital importance but remains challenging. Herein, a carbon nanotube‐supported single‐Sn‐atom catalyst (P‐SnN4‐CNT) is developed by a modified pyrolysis procedure with P‐doping into the second coordination shell of SnN4 moiety to modulate the electron structure of metal Sn center. The resulting P‐SnN4‐CNT delivered a high CO partial current density of −380 mA cm−2 with Faradaic efficiency (FE) of CO above 90% across a wide range of −0.5 to −0.8 V versus reversible hydrogen electrode (vs RHE), along with optimal FE (CO) of ≈98.5% at −0.6 V versus RHE in a flow cell. Moreover, P‐SnN4‐CNT achieved an extremely high turnover frequency of 126 471 h−1 with an applied potential of −0.8 V versus RHE, which ranks the best among the reported M─N─C catalysts for electrocatalytic CO2 reduction. The combination of in situ characterization techniques and density functional theory calculation revealed that the doping of P atoms benefited the activation and hydrogenation steps of CO2 and promoted the Sn4+ reduction to Sn2+ during the reaction process, where Sn2+ is identified as the active site for the CO generation. The work provides a clear mechanistic insight for both electron structure optimization and identification of active sites by local microenvironment regulation of single‐Sn‐atom, which shall pave a way for the exploitation of other M─N─C catalysts with high CO2RR performance.
期刊介绍:
Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small.
With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics.
The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.