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2024年2月20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《Two-dimensional peak-valley alternating self-supporting electrode accelerating nitrate electrocatalytic reduction: Ammonia synthesis and 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。
Abstract
Electrochemical nitrate reduction synthesis of ammonia can use clean energy to convert low-value nitrate pollutants into high value-added ammonia yield. The development of eNitRR catalyst with high activity, high selectivity and stability is the key to achieve distributed small-scale production of nitrate. In this study, a self-supported catalyst (Cu/PTS) with high catalytic activity (for eNitRR) was constructed by anodic oxidation combined with hydrothermal/pyrolysis strategy to realize the embedding of Cu species on the substrate of porous titanium sheet. The ammonia production rate of Cu/PTS catalyzed eNitRR is as high as 7292.43 μg h−1 cm−2 (−1.0 V vs. RHE), the Faradaic efficiency is close to 100 %, reaching 97.34 %, and isotope labeling and Operando ATR-FTIRAS verified and revealed the fact that NO3− to NH3, respectively. Density functional theory calculations well reveal the roles of various components in Cu/PTS and reveal the factors for the enhancement of eNitRR performance. Thanks to the self-supporting characteristics of porous titanium sheet and the surface embedding of copper species, Cu/PTS not only have good electrochemical stability when catalyzing eNitRR, but also can drive eNitRR to operate efficiently in complex water environment. While realizing the purification of nitrate wastewater and the synthesis of ammonia, Cu/PTS can be used as a positive electrode to construct a nitrate–zinc battery to realize the dual functions of self-driven ammonia production and external power supply.
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