Editable Hydrogen Bond Network Within the Electric Double Layer for CO <sub>2</sub> Reduction
Abstract
ABSTRACT The hydrogen bond network (HBN) of water is dynamic and highly sensitive to electrified interfaces, where its rigidity can be significantly altered. Tuning this property is crucial, as it directly impacts electrocatalytic performance and is a key requirement for scaling these processes industrially. In this study, the rigidity of the HBN within the electrical double layer (EDL) during electrolysis was edited by introducing different quaternary ammonium cations to a 1 M KHCO 3 buffer solution. CO 2 electroreduction was conducted using the different electrolytes, and the results reveal that the performance is highly dependent on the rigidity of the HBN within the EDL. A HBN with high rigidity favors CO production, whereas a HBN with low rigidity increases the formation of formate and H 2 . Notably, the production of C 2+ is maximized in an electrolyte where the HBN has moderate rigidity. By tuning the rigidity of the HBN, a Faradaic efficiency of 90.9% for C 2+ products is achieved with a current density of 0.81 A cm −2 over a typical Cu electrode. In situ spectroscopic and electrochemical measurements reveal that the rigidity of the HBN governs the configuration of the reaction intermediates and the kinetics of water dissociation, thereby dictating the final product distribution.
Article Details
Authors (19)
Jiahao Yang
Xiamen University , , ,
Shiju Yu
Beijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Sciences Beijing China
Jiapeng Jiao
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering
Shiqiang Liu
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry
Meng Zhou
Yiyong Wang
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry
Wenling Zhao
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry
Yaoyu Yin
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry
Hengan Wang
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry
Shipeng Zhang
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry
Zhongnan Ling
Beijing Synchrotron Radiation Facility
Huisheng Qin
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Centre for Excellence in Molecular Sciences, Centre for Carbon Neutral Chemistry
Ke Li
Xueqing Xing
Beijing Synchrotron Radiation Facility
Qinggong Zhu
Institute of Chemistry, Chinese Academy of Sciences , , ,
Yi Xu
Xiaofu Sun
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry
Xinchen Kang
Institute of Chemistry, Chinese Academy of Sciences , , ,
Buxing Han
Institute of Chemistry, Chinese Academy of Sciences , , ,