A Cu2B2 monolayer with planar hypercoordinate motifs: an efficient catalyst for CO electroreduction to ethanol
文献情報
Jingjing Jia, Haijun Zhang, Zhongxu Wang, Jingxiang Zhao, Zhen Zhou
Sustainable production of high-value carbon-based fuels and chemicals through electrochemical CO reduction (COR) under mild conditions is a promising alternative to the traditional Fischer–Tropsch process that requires high energy input and large-scale reactors. However, the COR process suffers from the low activity and poor selectivity of the currently employed electrocatalysts, greatly hampering its large-scale application. Herein, by means of comprehensive swarm-intelligence structure search and first-principles computations, we identify an ideal electrocatalyst for COR, i.e., a metallic Cu2B2 monolayer with planar heptacoordinate copper and planar pentacoordinate boron. Our results reveal that the predicted Cu2B2 monolayer exhibits superior thermal and dynamic stability and holds promise for experimental realization. More importantly, this catalyst could effectively reduce CO to ethanol through the “carbene” mechanism with a low limiting potential (−0.59 V) and a small barrier for C–C coupling (0.41 eV). Our work is the first report on the as-designed electrocatalyst with planar hypercoordinate motifs for CO reduction to C2 products, which not only widens the potential application of hypercoordinate 2D materials, but also opens up a new and promising avenue for converting abundant industrial CO to value-added ethanol.
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Journal of Materials Chemistry A, B & C cover high quality studies across all fields of materials chemistry. The journals focus on those theoretical or experimental studies that report new understanding, applications, properties and synthesis of materials. The journals have a strong history of publishing quality reports of interest to interdisciplinary communities and providing an efficient and rigorous service through peer review and publication. The journals are led by an international team of Editors-in-Chief and Associate Editors who are all active researchers in their fields. Journal of Materials Chemistry A, B & C are separated by the intended application of the material studied. Broadly, applications in energy and sustainability are of interest to Journal of Materials Chemistry A, applications in biology and medicine are of interest to Journal of Materials Chemistry B, and applications in optical, magnetic and electronic devices are of interest to Journal of Materials Chemistry C. More than one Journal of Materials Chemistry journal may be suitable for certain fields and researchers are encouraged to submit their paper to the journal that they feel best fits for their particular article. Example topic areas within the scope of Journal of Materials Chemistry A are listed below. This list is neither exhaustive nor exclusive. Artificial photosynthesis Batteries Carbon dioxide conversion Catalysis Fuel cells Gas capture/separation/storage Green/sustainable materials Hydrogen generation Hydrogen storage Photocatalysis Photovoltaics Self-cleaning materials Self-healing materials Sensors Supercapacitors Thermoelectrics Water splitting Water treatment










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