Mass transfer effect to electrochemical reduction of CO2: Electrode, electrocatalyst and electrolyte

Lu, Shun; Wang, Yucheng; Xiang, Hang; Lei, Hanhui; Xu, Ben Bin; Lü, Xing; Yu, Eileen Hao; Liu, Xiaoteng

doi:10.1016/j.est.2022.104764

Cited by 60 publications

(28 citation statements)

References 144 publications

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“…Overall, two K ions are chosen here to study the interfacial mechanisms of CO 2 RR and HER at Au–water interfaces. With explicit water solvents, cations, and negatively applied potential, the model system for CO 2 RR mechanistic study can be compared to the experimental condition with the commonly used aqueous electrolytes (NaHCO 3 or KHCO 3 , pH = 7.0) …”

Section: Introductionmentioning

confidence: 99%

“…With explicit water solvents, cations, and negatively applied potential, the model system for CO 2 RR mechanistic study can be compared to the experimental condition with the commonly used aqueous electrolytes (NaHCO 3 or KHCO 3 , pH = 7.0). 41 By constructing a solid−liquid interface to mimic the experimental condition, besides the CO 2 activation, the full reaction pathway including *CO 2 -to-*CO conversion and *CO desorption, is simulated via the slow-growth sampling method combined with ab initio molecular dynamics (SG-AIMD) simulations. Afterward, the complete free energy landscape is constructed to locate the rate-determining step (RDS), which is identified as the CO 2 activation reaction.…”

Section: ■ Introductionmentioning

confidence: 99%

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Cation-Coordinated Inner-Sphere CO₂ Electroreduction at Au–Water Interfaces

2023

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Electrochemical CO2 reduction reaction (CO2RR) is a promising technology for the clean energy economy. Numerous efforts have been devoted to enhancing the mechanistic understanding of CO2RR from both experimental and theoretical studies. Electrolyte ions are critical for the CO2RR; however, the role of alkali metal cations is highly controversial, and a complete free energy diagram of CO2RR at Au–water interfaces is still missing. Here, we provide a systematic mechanism study toward CO2RR via ab initio molecular dynamics simulations integrated with the slow-growth sampling (SG-AIMD) method. By using the SG-AIMD approach, we demonstrate that CO2RR is facile at the inner-sphere interface in the presence of K cations, which promote the CO2 activation with the free energy barrier of only 0.66 eV. Furthermore, the competitive hydrogen evolution reaction (HER) is inhibited by the interfacial cations with the induced kinetic blockage effect, where the rate-limiting Volmer step shows a much higher energy barrier (1.27 eV). Eventually, a comprehensive free energy diagram including both kinetics and thermodynamics of the CO2RR to CO and the HER at the electrochemical interface is derived, which illustrates the critical role of cations on the overall performance of CO2 electroreduction by facilitating CO2 adsorption while suppressing the hydrogen evolution at the same time.

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Section: Introductionmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

Cation-Coordinated Inner-Sphere CO₂ Electroreduction at Au–Water Interfaces

2023

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“…Recent advances in surface chemistry and spectroscopy also offer new opportunities to probe reaction mechanisms of CO 2 RR at the interfaces and, in turn, guide the design of such interfaces for catalysis enhancement. [122][123][124][125] Electrochemical systems that can be used to optimize gas transport, [126][127][128][129] electrolyte functions, [130][131][132][133] intermediate detection, [134][135][136][137][138][139] and reaction pathway engineering, [140][141][142] have been rapidly developed to improve the overall catalytic performance. In this section, we highlight how interfacial engineering can be applied to optimize electrolyte and catalyst surface ligand effects to enhance CO 2 RR catalysis.…”

Section: Catalyst-electrolyte Interface Engineering For Co 2 Reductionmentioning

confidence: 99%

Recent advances in CO₂ capture and reduction

et al. 2022

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“…The mass transfer limitation must be overcome to achieve an efficient eCO 2 RR at industrial-scale current density. 55,56 Hollow-fiber GPEs based on a gaseous CO 2 supply can improve the eCO 2 RR performance by circumventing CO 2 solubility limitations. Hollow fibers can optimize the kinetics in the eCO 2 RR owing to the higher CO 2 concentration at the electrode surface, the shorter transport paths, and a suitable porous substrate for gas diffusion.…”

Section: Co 2 Penetration Effectmentioning

confidence: 99%