多价MnOx/C电催化剂用于高效氮还原反应  

Polyvalent MnOx/C Electrocatalyst for Highly Efficient Nitrogen Reduction Reaction

作　　者：毕一飘 宫雪 杨发 阮明波[1] 宋平[1] 徐维林[1,2] BI Yipiao;GONG Xue;YANG Fa;RUAN Mingbo;SONG Ping;XU Weilin(Advanced Power Laboratory,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,China;University of Science and Technology of China,Hefei 230026,China)

机构地区：[1]中国科学院长春应用化学研究所,先进电源实验室,长春130022 [2]中国科学技术大学,合肥230026

出　　处：《应用化学》2020年第9期1048-1055,共8页Chinese Journal of Applied Chemistry

基　　金：国家杰出青年科学基金(21925205);广东联合基金(U1601211);国家自然科学基金(21733004,21633008,2017YF9127900,21721003,2018YFB1502302,21433003)项目资助。

摘　　要：氨在人类的生产生活中起着重要的作用,但目前工业上合成氨广泛采用的Haber-Bosch法耗能大,且污染严重。而N2电还原反应(ENRR)被认为是一种有效的替代方法,由于N2的键能较高,目前仍然缺乏高活性的催化剂。在这里,通过简单的浸渍法和氧化还原法制备了多价态的MnOx/C催化剂,该催化剂具有较高的氮还原反应活性(氨产率达到7.8μg NH3/(h·mg cat),法拉第效率高达9.2%)。进一步研究表明,多价态MnOx/C催化剂具有高氮还原反应活性的主要原因是不同价态的Mn离子(Mn^2+、Mn^3+、Mn^4+)之间存在协同效应。NH 3 plays an important role in human production and life,but the main way to produce NH 3 is still the high energy consumption and high pollution Haber-Bosch process.Electrocatalytic N2 reduction reaction(ENRR)is considered to be an effective alternative method,however highly efficient catalyst is still a challenging as a result of high bond energy of N■N.Here,we report an electrocatalyst of polyvalent MnOx/C which is designed via simple redox reaction for highly efficient production of ammonia(with yield up to 7.8μg NH 3/(h·mg cat)and Faradic efficiency(FE)up to 9.2%)from nitrogen reduction reaction(NRR).The high NRR performance of polyvalent MnO x/C mainly originates from a synergistic effect among different valence states(Mn^2+,Mn^3+,Mn^4+)of Mn for NRR.

关 键 词：合成氨 电催化 过渡金属氧化物 协同效应 

分 类 号：O646[理学—物理化学]