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2023年9月19日,Elsevier 旗下top期刊《Chemical Engineering Journal》在线发表了云南师范大学化学与化工学院高端引进人才赵学博士、赵焱教授、浙江海洋大学周英堂教授等团队合作的最新研究成果《Unlocking the potential of sub-nanometer-scale copper via confinement engineering: A remarkable approach for electrochemical nitrate-to-ammonia conversion in wastewater treatment》。第一作者单位为云南师范大学化学化工学院,浙江海洋大学为共同第一作者单位,第一作者为硕士研究生化学化工学院刘跃龙,赵学博士、赵焱教授和、浙江海洋大学周英堂教授为共同通讯作者。
Electrochemical-nitrate-reduction-reaction (eNitRR) ammonia synthesis shows the vision of green ammonia synthesis and is also an effective way to purify nitrate wastewater. In this study, the complex of 1,10-phenanthroline and Cu2+ was adsorbed on the surface of polydopamine-derived nitrogen-doped-hollow-carbon-spheres, and sub-nanometer-scale copper species (CuCN/NHCSs) were obtained after heat treatment. Using CuCN/NHCSs as catalyst, the ammonia yield rate and Faradaic efficiency of eNitRR reached 21413.5 μg h−1 mgcat.−1 (−1.1 V vs RHE) and 91.08% (−0.9 V vs RHE), respectively. CuCN/NHCSs still have high catalytic activity for eNitRR even in complex water environments (such as acidity, alkalinity, coexisting ions). In the face of low concentration of nitrate in natural sewage, CuCN/NHCSs as a catalyst can reduce the concentration of NO3− to below the limits set by WHO and US EPA within 10 h, and achieve effective purification of nitrate sewage. DFT calculations show that both single-atom Cu sites and Cu atom cluster sites on NHCSs can promote the electrochemical conversion of NO3− to ammonia, so minimizing copper sites can maximize the unit activity. Furthermore, the simultaneous anchoring of Cu atom clusters and single-atom Cu in the carbon matrix is beneficial to lower the energy barrier of the potential-determining step of eNitRR.
https://doi.org/10.1016/j.cej.2023.146176
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https://blog.sciencenet.cn/blog-454141-1393465.html
云南师范大学赵学博士在JOURNAL OF MATERIALS CHEMISTRY A上发表最新研究成果
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