原位重构限制在三维纳米孔铜内的铋纳米颗粒促电还原CO2
In situ reconstruction of Bi nanoparticles confined within 3D nanoporous Cu to boost CO2 electroreduction
赵秋玉 1王静 2庄严 1宫磊 1张薇宁 1樊唯镏 2鲁振 3张永政 4藤田武志 5张平 1薛其坤6
作者信息
- 1. School of Physics and Physical Engineering,Qufu Normal University,Qufu 273165,China
- 2. School of Chemistry and Chemical Engineering,Shandong University,Jinan 25010,China
- 3. Institute of Physics,Chinese Academy of Sciences,Beijing 100190,China
- 4. School of Physics and Physical Engineering,Qufu Normal University,Qufu 273165,China;Advanced Institute for Materials Research,Tohoku University,Sendai 980-8577,Japan
- 5. School of Environmental Science and Engineering,Kochi University of Technology,Kami 782-8502,Japan
- 6. Advanced Institute for Materials Research,Tohoku University,Sendai 980-8577,Japan
- 折叠
摘要
由于单金属Bi在CO2还原反应(CO2RR)中效率较低,通过表面工程复合材料提高电导率和产率是一种有吸引力的方法.在此,我们重构了在三维纳米孔铜结构中的原位生长金属Bi纳米颗粒.得益于三维纳米多孔导电网络和Cu与Bi之间的强相互作用,Bi@np-Cu费米能级向上移动,表现出优异的电催化二氧化碳还原性能.Bi@np-Cu在-0.97 V的电位下具有97.7%的甲酸法拉第效率,电流密度为82 mA cm-2.重要的是,该催化剂在连续催化反应40 h后仍能实现超过90%的法拉第效率.DFT计算表明,np-Cu有效地调节了Bi的电子态,优化了中间吸附能,从而提高了Bi的本征活性.这项工作为纳米多孔金属在催化中的应用提供了一个新视角.
Abstract
Due to the low efficiency of a single metal Bi in the CO2 reduction reaction(CO2RR)to formates,enhancing the conductivity and yield through surface engineered com-posites is an alluring approach.In this study,we reconstruct Bi nanoparticles in situ growth in 3D nanoporous copper struc-tures.Benefiting from the 3D nanoporous conductive network and the strong interaction between Cu and Bi,the Fermi level becomes shifted upward and the resulting Bi@np-Cu displays a surprising CO2RR performance.Bi@np-Cu demonstrates a formate faradaic efficiency of 97.7%at a potential of-0.97 V vs.reversible hydrogen electrode with a remarkable current density of 82 mA cm-2.Importantly,this catalyst also has a faradaic efficiency of more than 90%for a continuous CO2RR of 40 h.Density function theory calculations reveal that np-Cu effectively modulates the electronic states of Bi,optimizing the intermediate adsorption energy and leading to increased in-trinsic activity of Bi.This study provides a novel perspective on the applications of nanoporous metals in catalysis.
关键词
3D nanoporous/CO2RR/Bi nanoparticle/electro-catalysis/reconstructionKey words
3D nanoporous/CO2RR/Bi nanoparticle/electro-catalysis/reconstruction引用本文复制引用
基金项目
国家重点研发计划(2021YFB3802900)
国家自然科学基金重大项目(52192604)
Higher Educational Youth Innovation Science and Technology Program Shandong Province(2021KJ022)
山东省"泰山学者"项目(tsqn201909107)
山东省自然科学基金(ZR2020QF077)
国家自然科学基金(62104131)
Postdoctoral Science Foundation of Shandong Province(4456322)
出版年
2024