Switching CO <sub>2</sub> Electroreduction Pathways via Polyvinylpyrrolidone‐Mediated Water Configuration Control
Abstract
Abstract The water configuration plays a critical role in steering the CO 2 electroreduction pathway, yet achieving precise control over water arrangement remains a significant challenge. In this study, we demonstrate that introducing trace amounts of polyvinylpyrrolidone (PVP) into 3 M KCl enables targeted control over the CO 2 electroreduction product distribution by simply adjusting the PVP concentration. Using a Cu 19 CeO x (molar ratio of Cu:Ce = 19:1) electrode, in the absence of PVP, multicarbon (C 2+ ) products dominate, but substantial CO and H 2 are also generated, with negligible CH 4 formation. Remarkably, the addition of just 25 ppm PVP shifts the primary product to CH 4 , achieving a Faradaic efficiency (FE) of 60.4% at 500 mA cm −2 . Further increasing the PVP concentration to 125 ppm switches the dominant product back to C 2+ , with an impressive FE of 90.8% at 800 mA cm −2 . This trend is consistent across various Cu‐based catalysts, highlighting the universality of this approach. Mechanistic studies reveal that PVP reconstructs the water configuration at the cathode surface, modulating not only the adsorption strength and coverage of *CO intermediates but also the kinetics of water dissociation, thereby dictating the reaction pathway.
Article Details
Authors (16)
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
Zhongnan Ling
Beijing Synchrotron Radiation Facility
Keke Chai
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
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
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
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
Jiahao Yang
Xiamen University , , ,
Rongjuan Feng
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
Qingli Qian
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
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
Qinnggong Zhu
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 Institute of Chemistry Chinese Academy of Sciences Beijing China 100049
Yi Xu
Yongquan Zhou
Xinchen Kang
Institute of Chemistry, Chinese Academy of Sciences , , ,
Buxing Han
Institute of Chemistry, Chinese Academy of Sciences , , ,