Controlling the Selectivity of Electrocatalytic NO Reduction through pH and Potential Regulation on Single-Atom Catalysts

Qian, Sheng-Jie1,2; Cao, Hao1,2; Wang, Yang-Gang1,2; Li, Jun1,2,3,4

2024-04-25

10.1021/jacs.4c00827

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY   影响因子和分区

0002-7863

1520-5126

Electrocatalytic nitrogen oxide reduction (NOxRR) emerges as an effective way to bring the disrupted nitrogen cycle back into balance. However, efficient and selective NOxRR is still challenging partly due to the complex reaction mechanism, which is influenced by experimental conditions such as pH and electrode potential. Here, we have studied the enzyme-inspired iron single-atom catalysts (Fe-N4-C) and identified that the selectivity roots in the first step of the nitric oxide reduction. Combining the constrained molecular dynamics (MD) simulations with the quasi-equilibrium approximation, the effects of electrode potential and pH on the reaction free energy were considered explicitly and predicted quantitatively. Systematic heat maps for selectivity between single-N and N-N-coupled products in a wide pH-potential space are further developed, which have reproduced the experimental observations of NOxRR. The approach presented in this study allows for a realistic simulation of the electrocatalytic interfaces and a quantitative evaluation of interfacial effects. Our results in this study provide valuable and straightforward guidance for selective NOx reduction toward desired products by precisely designing the experimental conditions.

SCI

英语

第一 ; 通讯

Guangdong Provincial Pearl River Talents Program["22022504","220330005","22250710677"] ; National Natural Science Foundation of China (NSFC)[22388102] ; NSFC Center for Single-Atom Catalysis[2019QN01L353] ; Guangdong "Pearl River" Talent Plan["JCYJ20210324103608023","KCXST20221021111207017","JCYJ20220818100410023"]

Chemistry

Chemistry, Multidisciplinary

WOS:001227702300001

AMER CHEMICAL SOC

Web of Science

1.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Guangdong, Peoples R China
2.Southern Univ Sci & Technol, Guangdong Prov Key Lab Catalyt Chem, Shenzhen 518055, Guangdong, Peoples R China
3.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
4.Tsinghua Univ, Engn Res Ctr Adv Rare Earth Mat, Minist Educ, Beijing 100084, Peoples R China

Qian, Sheng-Jie,Cao, Hao,Wang, Yang-Gang,et al. Controlling the Selectivity of Electrocatalytic NO Reduction through pH and Potential Regulation on Single-Atom Catalysts[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2024,146(18).

Qian, Sheng-Jie,Cao, Hao,Wang, Yang-Gang,&Li, Jun.(2024).Controlling the Selectivity of Electrocatalytic NO Reduction through pH and Potential Regulation on Single-Atom Catalysts.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,146(18).

Qian, Sheng-Jie,et al."Controlling the Selectivity of Electrocatalytic NO Reduction through pH and Potential Regulation on Single-Atom Catalysts".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 146.18(2024).