Bao Yu Xia, Yingxi lin, Chenfeng xia, Zhaozhao Zhu, Junjie wang, Huiting Niu, Shuning Gong, Zhao Li, Na Yang, Junsong chen, rui Wu
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引用次数: 0
摘要
在膜电极组件(MEA)中设计高效的二氧化碳电还原催化剂面临着巨大的障碍。在此,我们提出了一种不对称配位的 Ni SAC,其特点是在 NiN4Br 位点上轴向配位 Br,并锚定在中空的 Br/N 共掺杂碳纳米笼上,通过 NaBr 辅助的约束-热解策略实现。在 MEA 器件中,Ni-NBr-C 在 50 到 350 mA cm-2 的电流密度范围内表现出很高的 CO 法拉第效率(FECO> 97%)。此外,Ni-NBr-C 的电池电压稳定在 2.66 ± 0.2 V,同时在 85 小时的长期运行中提供 350 mA cm-2 的大电流密度,这证明了它在工业规模应用中的潜力。先进的表征技术和理论计算表明,Br 的配位和掺杂提高了其内在活性,同时也突出表明独特的孔隙结构提高了传质效率。
Carbon Nanocage Supported Asymmetrically Coordinated Nickle Single-Atom for Enhanced CO2 Electroreduction in Membrane Electrode Assembly
Designing efficient catalysts for operating CO2 electroreduction in membrane electrode assembly (MEA) faces significant obstacles. Herein, we propose an asymmetrically coordinated Ni SAC featuring axial Br coordination at NiN4Br sites anchoring onto hollow Br/N co-doped carbon nanocages, achieved through a NaBr-assisted confined-pyrolysis strategy. The Ni-NBr-C exhibits a high CO Faradaic efficiency (FECO> 97%) over the current density range of 50 to 350 mA cm−2 in the MEA device. Furthermore, Ni-NBr-C shows a stable cell voltage of 2.66 ± 0.2 V while delivering a large current density of 350 mA cm−2 over an 85-hour long-term operation, demonstrating its potential for industrial-scale applications. Advanced characterization techniques and theoretical calculations reveal that the coordination and doping of Br enhance the intrinsic activity but also highlighted that the unique pore structure improves mass transfer efficiency.
期刊介绍:
Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.