揭示多金属氧化物各元素协同作用实现硝酸根高效还原为氨

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中文摘要：电催化硝酸根还原反应(NO3-RR)被认为是一种有前景且可持续的氨(NH3)合成新方法,但生成NH3的选择性和产率受到析氢副反应和复杂八电子转移过程的限制.本文开发了一种(FeCoNiCu)Ox/CeO2多金属氧化物电催化剂,能够将NO3-高效还原为NH3.文章通过设计系列实验,揭示了催化剂中不同元素之间的协同作用:Cu作为活性位点用于将NO3-还原为NO2-,Co作为中继位点促进NO2-进一步还原为NH3,Fe和Ni则通过加速水解离保证了反应所需的质子供应.此外,CeO2的加入显著增加了(FeCoNiCu)Ox多金属氧化物的活性表面积,进而提高了NH3产率.最终,(FeCoNiCu)Ox/CeO2电e催化剂实现了高的NH3电流密度(382 mA cm-2)和NH3产率(30.3 mg h-1 cm-2),兼具优异的长期稳定性.本项工作推动了多元素氧化物在电催化领域的应用,为高效多元素电催化剂的设计提供了有价值的见解.

外文标题：Unveiling multi-element synergy in polymetallic oxides for efficient nitrate reduction to ammonia

外文摘要：Electrocatalytic nitrate reduction reaction is considered as a promising and sustainable method for am-monia synthesis.However,the selectivity and yield rate of ammonia are limited by the competitive hydrogen evolution reaction and the complex eight-electron transfer process.Herein,we developed a(FeCoNiCu)Ox/CeO2 polymetallic oxide electrocatalyst for effective nitrate reduction to ammo-nia.The synergistic effects among the multiple elements in the electrocatalyst were clearly elucidated by comprehensive ex-periments.Specifically,Cu acted as the active site for reducing nitrate to nitrite,and Co facilitated the subsequent reduction of nitrite to ammonia,while Fe and Ni promoted water dis-sociation to provide protons.Furthermore,the incorporation of CeO2 increased the active surface area of(FeCoNiCu)Ox,resulting in an improved ammonia yield rate to meet in-dustrial demands.Consequently,the(FeCoNiCu)Ox/CeO2 electrocatalyst achieved an ammonia current density of 382 mA cm-2 and a high ammonia yield rate of 30.3 mg h-1 cm-2 with a long-term stability.This work offers valuable insights for the future design of highly efficient multi-element elec-trocatalysts.

外文关键词：

multi-element synergyelectrocatalysisammonia synthesispolymetallic oxidesrapid Joule-heating method

作者：

郄亚宁、高嘉辰、李思琪、崔铭锦、毛雪娇、王新宇、张渤、池思伽、贾怡然、杨全红、杨春鹏、翁哲

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作者单位：

Nanoyang Group,Tianjin Key Laboratory of Advanced Carbon and Electrochemical Energy Storage,School of Chemical Engineering and Technology,and Collaborative Innovation Center of Chemical Science and Engineering(Tianjin),Tianjin University,Tianjin 300072,China

National Industry-Education Integration Platform of Energy Storage,Tianjin University,Tianjin 300072,China

Haihe Laboratory of Sustainable Chemical Transformations,Tianjin 300192,China

Institute of Energy Materials Science,University of Shanghai for Science and Technology,Shanghai 200093,China

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关键词：

multi-element synergy electrocatalysis ammonia synthesis polymetallic oxides rapid Joule-heating method

基金：

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNatural Science Foundation of TianjinNational Industry-Education Integration Platform of Energy StorageFundamental Research Funds for the Central UniversitiesHaihe Laboratory of Sustainable Chemical Transformations

项目编号：

519722235220227920JCYBJC01550

出版年：

2024

DOI：

10.1007/s40843-024-3017-4

中国科学:材料科学(英文)

CSTPCD

ISSN：

年,卷(期)：2024.67(9)