贝壳状Ni_(3)S_(2)/NiMoP_(2)异质结构电催化剂高效大电流密度电解水/尿素复合系统  

Shell-shaped Ni_(3)S_(2)/NiMoP_(2) hetero-structure electrocatalyst for efficient water-urea electrolysis at high current density

作　　者：王佳奕 庆绍军 童希立[3] 项婷 张坤[1] 徐良骥[1,2] WANG Jiayi;QING Shaojun;TONG Xili;XIANG Ting;ZHANG Kun;XU Liangji(School of Earth and Environment,Anhui University of Science and Technology,Huainan 232001,China;School of Carbon Neutrality Science and Engineering,Anhui University of Science and Technology,Hefei 231131,China;State Key Laboratory of Coal Conversion,Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,China;Institute of Energy,Hefei Comprehensive National Science Center(Anhui Energy Laboratory),Hefei 230026,China)

机构地区：[1]安徽理工大学地球与环境学院,安徽淮南232001 [2]安徽理工大学碳中和科学与工程学院,安徽合肥231131 [3]中国科学院山西煤炭化学研究所煤炭高效低碳利用全国重点实验室,山西太原030001 [4]合肥综合性国家科学中心能源研究院(安徽省能源实验室),安徽合肥230026

出　　处：《燃料化学学报(中英文)》2025年第1期116-127,共12页Journal of Fuel Chemistry and Technology

基　　金：安徽理工大学高层次引进人才科研启动基金(2023yjrc51);安徽省科技厅(2022h11020024);安徽建工集团有限公司(SG2025Q11);煤炭高效低碳利用全国重点实验室开放课题基金(J24-25-603);中国科学院山西煤炭化学研究所基础研究项目(SCJC-HN-2022-17);山西省科学基金(20210302124446,2012102070301018);安徽省高校协同创新计划项目(GXXT-2022-27)资助。

摘　　要：水-尿素电解是实现氨氮废水脱氮及高效绿色产氢的有效途径之一,但该技术面临的关键难题是缺乏高活性和大电流耐久性的双功能电催化剂。本研究采用水热耦合气相磷化法,在泡沫镍(NF)上合成了一种贝壳状Ni_(3)S_(2)/NiMoP_(2)异质结构催化剂,得益于其片状层叠的非均相纳米结构、丰富的氧空位和高效的电子传质,该电催化剂在析氢反应(HER)和尿素氧化反应(UOR)中表现出优异的活性,产生1000 mA/cm^(2)的大电流密度分别仅需−0.205和1.423 V(vs.RHE)的超低电位。双功能Ni_(3)S_(2)/NiMoP_(2)催化剂组装的水-尿素系统的电解活性得到显著提升,仅需要1.580 V的槽压来驱动500 mA/cm^(2)电流密度实现HER和UOR,比全水解系统的电压低159 mV。此外,它在高电流条件下表现出优异的耐久性,可以连续稳定运行长达100 h。Water-urea electrolysis represents a promising avenue for nitrogen removal and efficient green hydrogen production from ammonia nitrogen wastewater.However,a key challenge,viz.,the lack of bifunctional electrocatalysts with exceptional activity and long-term current stability toward hydrogen evolution reaction(HER)and urea oxidation reaction(UOR),lies in this avenue.In this regard,a shell-shaped Ni_(3)S_(2)/NiMoP_(2) heterostructure was constructed on nickel foam(NF)by a hydrothermal method coupled with the gas phase phosphating.Thanks to its laminated heterogeneous nanostructure with abundant oxygen vacancy and efficient electron mass transfer,this catalyst displays excellent activity both in HER and in UOR,with an ultra-low potential of−0.205 and 1.423 V(vs.RHE),respectively,to achieve a large current density of 1000 mA/cm^(2).The dual-electrode water-urea system assembled with the bifunctional Ni_(3)S_(2)/NiMoP_(2) catalyst requires only 1.580 V to achieve a current density of 500 mA/cm^(2),which is 159 mV lower than that in the overall water splitting.Additionally,it exhibits great durability and can operate stably and continuously for up to 100 h under high current conditions.

关 键 词：Ni_(3)S_(2)/MoNiP_(2) 异质结构 电催化剂 尿素氧化 制氢 

分 类 号：O643.36[理学—物理化学]