摘要
硝酸根还原反应(NtRR)是一种合成氨(NH3)的有效方法。催化剂的合成包括2步简单的工艺:首先在炭布(CC)上合成Co_(3)O_(4)纳米线,然后以六乙炔基苯(HEB)为前驱体在Co_(3)O_(4)表面生长石墨炔(GDY)(110°C, 10 h),从而可控合成Co_(3)O_(4)/GDY纳米线异质结催化剂。高分辨率扫描电镜(SEM)、透射电镜(HRTEM)、X射线光电子能谱(XPS)和拉曼表征等证实了Co_(3)O_(4)/GDY异质界面的成功合成,界面处形成的独特的sp-C―Co键以及GDY与Co之间的不完全电荷转移为催化反应提供了持续的电子供应,保证了NtRR的高效进行。Co_(3)O_(4)/GDY在NtRR中展现了优异催化性能,其NH_(3)产率(YNH3)和法拉第效率(FE)分别达到了0.78 mmol h^(-1)cm^(-2)和92.45%。这项工作为在温和条件下,从废水中高性能生产氨的异质结构提供了一种通用方法。
The nitrate reduction reaction(NtRR)has been demonstrated to be a promising way for obtaining ammonia(NH_(3))by converting NO3-to NH3.Here we report the controlled synthesis of cobalt tetroxide/graphdiyne heterostructured nanowires(Co_(3)O_(4)/GDY NWs)by a simple two-step process including the synthesis of Co_(3)O_(4) NWs and the following growth of GDY using hex-aethynylbenzene as the precursor at 110°C for 10 h.Detailed scanning electron microscopy,high resolution transmission electron microscopy,X-ray photoelectron spectroscopy,and Raman characterization confirmed the synthesis of a Co_(3)O_(4)/GDY heterointerface with the formation of sp-C-Co bonds at the interface and incomplete charge transfer between GDY and Co,which provide a con-tinuous supply of electrons for the catalytic reaction and ensure a rapid NtRR.Because of these advantages,Co_(3)O_(4)/GDY NWs had an excellent NtRR performance with a high NH3 yield rate(YNH3)of 0.78 mmol h^(-1) cm^(-2) and a Faraday efficiency(FE)of 92.45% at-1.05 V(vs.RHE).This work provides a general approach for synthesizing heterostructures that can drive high-performance ammo-nia production from wastewater under ambient conditions.
作者
陈朝阳
赵淑雅
栾晓雨
郑志强
闫佳玉
薛玉瑞
CHEN Zhao-yang;ZHAO Shu-ya;LUAN Xiao-yu;ZHENG Zhi-qiang;YAN Jia-yu;XUE Yu-rui(Shandong Provincial Key Laboratory for Science of Material Creation and Energy Conversion,Science Center for Material Creation and Energy Conversion,School of Chemistry and Chemical Engineering,Shandong University,Jinan 250100,China)
出处
《新型炭材料（中英文）》
SCIE
EI
CAS
CSCD
北大核心
2024年第1期142-151,共10页
New Carbon Materials
基金
国家重点研发计划项目(2022YFA1204500,2022YFA1204501,2022YFA1204503,2018YFA0703501)
山东省泰山学者青年专家项目(tsqn201909050)
山东省自然科学基金(ZR2020ZD38,ZR2021JQ07).
关键词
石墨炔
异质结构
电催化
硝酸根还原反应
制氨
Graphdiyne
Heterostructures
Electrocatalysis
Nitrate reduction reaction
Ammonia production
