Tip‐Induced Self‐Enhanced Concentration Gradients Catalyst for Sustainable Electrocatalytic Urea Synthesis
Abstract
ABSTRACT Electrocatalytic C─N coupling via the co‐reduction of CO 2 and NO 3 − represents a promising route for sustainable urea synthesis under ambient conditions, simultaneously addressing critical challenges in energy sustainability and environmental remediation. However, its practical implementation is hindered by sluggish C─N coupling kinetics and the competing hydrogen evolution reaction (HER), which severely restricts energy conversion efficiency. Herein, we propose a tip‐induced local electric field strategy that generates a self‐enhanced concentration gradient to promote electrocatalytic C─N coupling. By constructing densely aligned Co 3 O 4 nanoneedles on carbon cloth, an outstanding electrocatalytic performance was achieved, requiring only an ultra‐low potential of −0.60 V versus reversible hydrogen electrode (RHE) while delivering a high urea yield rate of 49.63 umol h −1 cm −2 and a Faradic efficiency of 21.37%. Finite element simulations reveal that the nanoscale high‐curvature tip generates an intensified local electric field, enriching potassium ions (K + ) at the electrode‐electrolyte interface to stabilize key intermediates and direct the reaction pathway toward C─N coupling. Moreover, a series of operando spectroscopic characterizations provide direct evidence for enhanced C─N coupling process under an intensified local electric field. This work offers a generalizable strategy for energy‐efficient C─N coupling, paving the way for sustainable utilization of nitrogen and carbon resources.
Article Details
Authors (18)
Mingyu Chen
Xupeng Qin
National Synchrotron Radiation Laboratory
Nannan Guo
State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources College of Chemistry Xinjiang University Urumqi China
Zhou Chen
Australian Institute for Bioengineering and Nanotechnology
Chu Zhang
MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, State Key Laboratory of Space Power-Sources, School of Chemistry and Chemical Engineering
Lipan Luo
State Key Laboratory of Chemo and Biosensing College of Chemistry and Chemical Engineering International Joint Lab of Energy Electrochemistry of the Ministry of Education Hunan University Changsha P. R. China
Kaizhi Gu
Institute for Advanced Study
Chade Lv
MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, State Key Laboratory of Space Power-Sources, School of Chemistry and Chemical Engineering
Luxiang Wang
State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources College of Chemistry Xinjiang University Urumqi China
Qinghua Liu
National Synchrotron Radiation Laboratory
Zhong Cheng
State Key Laboratory of Chemo and Biosensing, College of Chemistry and Chemical Engineering, Advanced Catalytic Engineering Research Center of the Ministry of Education
Ze Wu
Han Li
Yidan Huo
State Key Laboratory of Chemo and Biosensing College of Chemistry and Chemical Engineering International Joint Lab of Energy Electrochemistry of the Ministry of Education Hunan University Changsha P. R. China
Dawei Chen
State Key Laboratory of Chemo and Biosensing, College of Chemistry and Chemical Engineering, Advanced Catalytic Engineering Research Center of the Ministry of Education
Guobin Wen
State Key Laboratory of Chemo and Biosensing, College of Chemistry and Chemical Engineering
Chen Chen
Shuangyin Wang
State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering