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
Unveiling multi-element synergy in polymetallic oxides for efficient nitrate reduction to ammonia
郄亚宁 1高嘉辰 1李思琪 1崔铭锦 2毛雪娇 1王新宇 1张渤 1池思伽 1贾怡然 1杨全红 1杨春鹏 1翁哲1
作者信息
- 1. 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
- 2. Institute of Energy Materials Science,University of Shanghai for Science and Technology,Shanghai 200093,China
- 折叠
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.
Abstract
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.
关键词
multi-element synergy/electrocatalysis/ammonia synthesis/polymetallic oxides/rapid Joule-heating methodKey words
multi-element synergy/electrocatalysis/ammonia synthesis/polymetallic oxides/rapid Joule-heating method引用本文复制引用
基金项目
National Natural Science Foundation of China(51972223)
National Natural Science Foundation of China(52202279)
Natural Science Foundation of Tianjin(20JCYBJC01550)
National Industry-Education Integration Platform of Energy Storage()
Fundamental Research Funds for the Central Universities()
Haihe Laboratory of Sustainable Chemical Transformations()
出版年
2024
NETL
NSTL
万方数据