Jiayu Li

Bio: Jiayu Li is an academic researcher from East China University of Science and Technology. The author has contributed to research in topics: Catalysis & Electron transfer. The author has an hindex of 4, co-authored 6 publications receiving 47 citations.

Structure‐Tunable Copper–Indium Catalysts for Highly Selective CO2 Electroreduction to CO or HCOOH

Abstract: Selectively approaching chemicals with one composition-tunable catalyst is attractive for practical manufacturing. Bimetallic copper-indium (Cu-In) catalysts have been synthesized by using a coprecipitation method and found to be among the best reported In-based catalysts for electrochemical CO2 reduction to CO or HCOOH. By varying the metal ratio, the catalyst can be tuned from a core-shell structure that selectively produces CO to a well-mixed structure that prefers HCOOH production. The distinct selectivities depend on the structure-sensitive binding strength of key reactive intermediates. These findings can benefit the development of a broader range of selectivity-tunable catalysts.

Probing the role of surface hydroxyls for Bi, Sn and In catalysts during CO2 Reduction

Abstract: Electrodeposited Bi, Sn and In catalysts are employed as model catalysts to investigate the nature of active sites and the influence of surface hydroxyls on the formation of formate during CO2 electroreduction (CO2RR). With SEM, XPS, in situ XRD, electrochemical measurements and DFT calculations, the active sites are Bi0, SnO and In2O3, with their affinities to hydroxyls following the trend of Bi0

Recent Advances in Electrochemical CO2 Reduction on Indium-Based Catalysts

Abstract: Electrochemical reduction of CO2 (CO2RR) is a promising solution to mitigate the ever‐increasing global carbon emission. Indium‐based catalysts have been extensively studied for catalyzing the production of formate, CO, and even multi‐carbon molecules from CO2. Rational design of the catalyst, however, is urgently needed to further improve the activity, selectivity, and stability for the sake of commercialization. Herein, we comprehensively reviewed recent progresses on the indium based CO2RR catalysts. Specifically, aspects regarding the nature of active sites, reaction mechanism, and the impact of operating conditions are overviewed. The reported indium‐based monometallic and bimetallic catalysts in the literature are summarized, as well. Future directions should be focused on the understanding of catalyst system during the reaction and under industrial‐relevant conditions.

Structure–Activity Relationship of the PolymerizedCobalt Phthalocyanines for Electrocatalytic Carbon Dioxide Reduction

Abstract: Polymeric frameworks composed of molecular complexes have been attractive for the outstanding activity, selectivity, and stability toward CO2-to-CO conversion. In this work, polymerized cobalt phthalocyanines (CoPPc) with different functionalities were investigated with a series of spectroscopy characterizations, controlled-potential electrolysis, Tafel analysis, cyclic voltammetry analysis, and isotope labeling studies. The electronic structure of the Co center was revealed to be directly affected by the peripheral substituents via an inductive effect. Besides, the relationship between electronic structure and activity of the CoPPc-based catalysts for CO2 electroreduction was successfully elucidated at the molecular level.

Electrocatalysis for CO2 conversion: from fundamentals to value-added products

Abstract: The continuously increasing CO2 released from human activities poses a great threat to human survival by fluctuating global climate and disturbing carbon balance among the four reservoirs of the biosphere, earth, air, and water. Converting CO2 to value-added feedstocks via electrocatalysis of the CO2 reduction reaction (CO2RR) has been regarded as one of the most attractive routes to re-balance the carbon cycle, thanks to its multiple advantages of mild operating conditions, easy handling, tunable products and the potential of synergy with the rapidly increasing renewable energy (i.e., solar, wind). Instead of focusing on a special topic of electrocatalysts for the CO2RR that have been extensively reviewed elsewhere, we herein present a rather comprehensive review of the recent research progress, in the view of associated value-added products upon selective electrocatalytic CO2 conversion. We initially provide an overview of the history and the fundamental science regarding the electrocatalytic CO2RR, with a special introduction to the design, preparation, and performance evaluation of electrocatalysts, the factors influencing the CO2RR, and the associated theoretical calculations. Emphasis will then be given to the emerging trends of selective electrocatalytic conversion of CO2 into a variety of value-added products. The structure-performance relationship and mechanism will also be discussed and investigated. The outlooks for CO2 electrocatalysis, including the challenges and opportunities in the development of new electrocatalysts, electrolyzers, the recently rising operando fundamental studies, and the feasibility of industrial applications are finally summarized.

Rational Catalyst and Electrolyte Design for Co2 Electroreduction Towards Multicarbon Products

Abstract: CO2 electroreduction reaction (CO2RR) to fuels and feedstocks is an attractive route to close the anthropogenic carbon cycle and store renewable energy. The generation of more reduced chemicals, especially multicarbon oxygenate and hydrocarbon products (C2+) with higher energy density is highly desirable for industrial applications. However, selective conversion of CO2 to C2+ suffers from high overpotential, low reaction rate and low selectivity, and the process is extremely sensitive to the catalyst structure and electrolyte. Here we discuss strategies to achieve high C2+ selectivity through rational design of the catalyst and electrolyte. Current state-of-the-art catalysts, including Cu and Cu-bimetallic catalysts as well as alternative materials are considered. The importance of taking into consideration the dynamic evolution of the catalyst structure and composition are highlighted, focusing on findings extracted from in situ and operando characterizations. Additional theoretical insight into the reaction mechanisms underlying the improved C2+ selectivity of specific catalyst geometries/compositions in synergy with a well-chosen electrolyte are also provided.

Transition metal-based catalysts for the electrochemical CO2 reduction: from atoms and molecules to nanostructured materials

Abstract: The electrochemical reduction of carbon dioxide (CO2) powered by renewable energy is an attractive sustainable approach to mitigate CO2 emissions and to produce fuels or value-added chemicals. In order to tackle the challenges related to selectivity, activity, overpotential and durability, transition metal-based catalysts have been widely investigated in the last decades. In an effort to bridge the gap between the fields of homogeneous and heterogeneous catalysis, this review aims to survey the main strategies explored for the rational design of a wide variety of different metal catalysts, ranging from molecular systems to single-atom and nanostructured catalysts. Transition metal complexes containing heme and non-heme ligands have been selected to discuss the recent advances in the understanding of the structure–function relationship in molecular homogeneous catalysis as well as to summarize the main approaches proposed for the heterogenization or confinement of molecular catalysts on conductive surfaces. The main strategies to minimize catalyst cost are also presented, leading to atomically dispersed molecular-like M–Nx moieties embedded on 2D conducting materials. The superior performances of single-atom catalysts (SACs) and the structural similarity with their molecular analogs, suggest that transition metal catalysts containing well-defined sites may be intrinsically more active and selective towards CO2 conversion than the bulk heterogeneous materials. Finally, design approaches for metal nanoparticles (NPs) based on size, shape, and support tuning are summarized and compared to novel strategies based on the interaction with surface-bonded organic molecules. The studies herein presented show that the basic principles in molecular catalysis and organometallic chemistry can be effectively used to design new efficient and selective heterogeneous catalysts for CO2 reduction.

An industrial perspective on catalysts for low-temperature CO2 electrolysis

Abstract: Electrochemical conversion of CO2 to useful products at temperatures below 100 °C is nearing the commercial scale. Pilot units for CO2 conversion to CO are already being tested. Units to convert CO2 to formic acid are projected to reach pilot scale in the next year. Further, several investigators are starting to observe industrially relevant rates of the electrochemical conversion of CO2 to ethanol and ethylene, with the hydrogen needed coming from water. In each case, Faradaic efficiencies of 80% or more and current densities above 200 mA cm−2 can be reproducibly achieved. Here we describe the key advances in nanocatalysts that lead to the impressive performance, indicate where additional work is needed and provide benchmarks that others can use to compare their results. This Perspective describes the key advances in nanocatalysts that have led to the impressive electrochemical conversion of CO2 to useful products and provides benchmarks that others can use to compare their results.

Gas diffusion electrodes (GDEs) for electrochemical reduction of carbon dioxide, carbon monoxide, and dinitrogen to value-added products: a review

Abstract: Electrochemical reduction of gaseous feeds such as CO2, CO, and N2 holds promise for sustainable energy and chemical production. Practical application of this technology is impeded by slow mass transport of the sparingly soluble gases to conventional planar electrodes. Gas diffusion electrodes (GDEs) maintain a high gas concentration in the vicinity of the catalyst and improve mass transport, thereby resulting in current densities higher by orders of magnitude. However, gaseous feeds cause changes to the GDE environment, and specific features are required to efficiently tune the product selectivity and improve reaction stability. Herein, with a comprehensive review of the challenges and advances in GDE development for various electrocatalytic reactions, we intend to complement the body of material-focused reviews. This review outlines GDE fundamentals and highlights key advantages of GDE over conventional electrodes. Through critical discussion about steps in GDE fabrication, and specific shortcomings and remedial strategies for various electrochemical applications, this review discusses connections, unique design criteria, and potential opportunities for gas-fed reactions and desired products. Finally, priorities for future studies are suggested, to support the advancement and scale-up of GDE-based electrochemical technologies.