ORCID Profile
0000-0001-9387-3465
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Publisher: American Chemical Society (ACS)
Date: 21-10-2021
Publisher: Wiley
Date: 16-10-2021
Publisher: Wiley
Date: 07-07-2021
Abstract: Monitoring and controlling the reconstruction of materials under working conditions is crucial for the precise identification of active sites, elucidation of reaction mechanisms, and rational design of advanced catalysts. Herein, a Bi‐based metal–organic framework (Bi‐MOF) for electrochemical CO 2 reduction is selected as a case study. In situ Raman spectra combined with ex situ electron microscopy reveal that the intricate reconstruction of the Bi‐MOF can be controlled using two steps: 1) electrolyte‐mediated dissociation and conversion of Bi‐MOF to Bi 2 O 2 CO 3 , and 2) potential‐mediated reduction of Bi 2 O 2 CO 3 to Bi. The intentionally reconstructed Bi catalyst exhibits excellent activity, selectivity, and durability for formate production, and the unsaturated surface Bi atoms formed during reconstruction become the active sites. This work emphasizes the significant impact of pre‐catalyst reconstruction under working conditions and provides insight into the design of highly active and stable electrocatalysts through the regulation of these processes.
Publisher: American Chemical Society (ACS)
Date: 05-10-2023
Publisher: Wiley
Date: 09-07-2021
Abstract: Monitoring and controlling the reconstruction of materials under working conditions is crucial for the precise identification of active sites, elucidation of reaction mechanisms, and rational design of advanced catalysts. Herein, a Bi‐based metal–organic framework (Bi‐MOF) for electrochemical CO 2 reduction is selected as a case study. In situ Raman spectra combined with ex situ electron microscopy reveal that the intricate reconstruction of the Bi‐MOF can be controlled using two steps: 1) electrolyte‐mediated dissociation and conversion of Bi‐MOF to Bi 2 O 2 CO 3 , and 2) potential‐mediated reduction of Bi 2 O 2 CO 3 to Bi. The intentionally reconstructed Bi catalyst exhibits excellent activity, selectivity, and durability for formate production, and the unsaturated surface Bi atoms formed during reconstruction become the active sites. This work emphasizes the significant impact of pre‐catalyst reconstruction under working conditions and provides insight into the design of highly active and stable electrocatalysts through the regulation of these processes.
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1EE00740H
Abstract: The review presents the important role of oxygen-bound intermediates in directing the selectivity of electrochemical CO 2 reduction by considering available theoretical calculations, electrochemical measurements and operando spectroscopy observations.
Publisher: American Chemical Society (ACS)
Date: 04-08-2022
DOI: 10.1021/JACS.2C06820
Abstract: An ere-level current density of CO
Publisher: Wiley
Date: 25-05-2020
Abstract: Electrochemical conversion of CO 2 into ethane is seldom observed because of the generally higher selectivity towards methane, ethylene, and ethanol. Consequently, little experimental evidence for its reaction mechanism exists and thus remains largely unknown. Now, by combining electrochemistry with in situ X‐ray absorption fine‐structure and in situ Raman techniques, iodide‐derived copper (ID‐Cu) and oxide‐derived copper (OD‐Cu) systems were studied to obtain a deeper understanding of the CO 2 to ethane mechanism. With trace iodine species on the surface and positively charged Cu species, production of ethane is significantly more favored on ID‐Cu compared to OD‐Cu, with higher selectivity and faster kinetics. For the first time, it is experimentally found that the formation of ethane follows the same pathway to ethylene and ethanol, and better stabilization of the late stage ethoxy intermediate can steer the reaction to ethane over ethanol.
Publisher: Elsevier BV
Date: 10-2023
Publisher: Springer Science and Business Media LLC
Date: 02-01-2023
Publisher: American Chemical Society (ACS)
Date: 05-09-2019
Publisher: Wiley
Date: 18-01-2021
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1CC03796J
Abstract: The OC–COH coupling is kinetically facilitated compared to OC–CHO coupling, which is induced by the optimized composition and electronic structures of copper alloys.
Publisher: Wiley
Date: 06-02-2022
Abstract: Dual‐atom catalysts (DACs) have become an emerging platform to provide more flexible active sites for electrocatalytic reactions with multi‐electron roton transfer, such as the CO 2 reduction reaction (CRR). However, the introduction of asymmetric dual‐atom sites causes complexity in structure, leaving an incomprehensive understanding of the inter‐metal interaction and catalytic mechanism. Taking NiCu DACs as an ex le, herein, a more rational structural model is proposed, and the distance‐dependent inter‐metal interaction is investigated by combining theoretical simulations and experiments, including density functional theory computation, aberration‐corrected transmission electron microscopy, synchrotron‐based X‐ray absorption fine structure, and Monte Carlo experiments. A distance threshold around 5.3 Å between adjacent NiN 4 and CuN 4 moieties is revealed to trigger effective electronic regulation and boost CRR performance on both selectivity and activity. A universal macro‐descriptor rigorously correlating the inter‐metal distance and intrinsic material features (e.g., metal loading and thickness) is established to guide the rational design and synthesis of advanced DACs. This study highlights the significance of identifying the inter‐metal interaction in DACs, and helps bridge the gap between theoretical study and experimental synthesis of atomically dispersed catalysts with highly correlated active sites.
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D0TA11604A
Abstract: Understanding the late stages of C 2 pathways provides great opportunities for fully achieving a selective CO 2 electroreduction. The C 2 product selectivity can be directed by the active site's oxygen affinity on a range of non-metal doped Cu surfaces.
Publisher: Elsevier BV
Date: 05-2020
Publisher: Wiley
Date: 15-11-2022
Abstract: Photocatalytic performance can be optimized via introduction of reactive sites. However, it is practically difficult to engineer these on specific photocatalyst surfaces, because of limited understanding of atomic‐level structure‐activity. Here we report a facile sonication‐assisted chemical reduction for specific facets regulation via oxygen deprivation on Bi‐based photocatalysts. The modified Bi 2 MoO 6 nanosheets exhibit 61.5 and 12.4 μmol g −1 for CO and CH 4 production respectively, ≈3 times greater than for pristine catalyst, together with excellent stability/reproducibility of ≈20 h. By combining advanced characterizations and simulation, we confirm the reaction mechanism on surface‐regulated photocatalysts, namely, induced defects on highly‐active surface accelerate charge separation/transfer and lower the energy barrier for surface CO 2 adsorption/activation/reduction. Promisingly, this method appears generalizable to a wider range of materials.
Publisher: Wiley
Date: 04-02-2019
Abstract: Effective electrocatalysts are required for the CO
Publisher: Wiley
Date: 15-01-2022
Abstract: Aqueous zinc batteries, that demonstrate high safety and low cost, are considered promising candidates for large‐scale energy storage. However, Zn anodes suffer from rapid performance deterioration due to the severe Zn dendrite growth and side reactions. Herein, with a low‐cost ammonium acetate (NH 4 OAc) additive, a self‐regulated Zn/electrolyte interface is built to address these problems. The NH 4 + induces a dynamic electrostatic shielding layer around the abrupt Zn protuberance to make the Zn deposition uniform, and the OAc − acts as an interfacial pH buffer to suppress the proton‐induced side reactions and the precipitation of insoluble by‐products. As a result, in the electrolyte with the NH 4 OAc additive, Zn anodes exhibit a long cycling stability of 3500 h at 1 mA cm −2 , an impressive cumulative areal capacity of 5000 mAh cm −2 at 10 mA cm −2 , and a high Coulombic efficiency of ≈ 99.7%. A prototype full cell coupled with a NH 4 V 4 O 10 cathode performs much better in terms of capacity retention than the additive‐free case. The findings pave the way for developing practical Zn batteries.
No related grants have been discovered for Xing Zhi.