Selective CO2‐to‐Syngas Conversion Enabled by Bimetallic Gold/Zinc Sites in Partially Reduced Gold/Zinc Oxide Arrays DOI
Ruirui Zhao,

Ziyin Zhu,

Ting Ouyang

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(6)

Published: Oct. 19, 2023

Abstract Electrocatalytic CO 2 ‐to‐syngas (gaseous mixture of and H ) is a promising way to curb excessive emission the greenhouse gas effect. Herein, we present bimetallic AuZn@ZnO (AuZn/ZnO) catalyst with high efficiency durability for electrocatalytic reduction O, which enables Faradaic 66.4 % 26.5 3 h stability at −0.9 V vs. reversible hydrogen electrode (RHE). The CO/H ratios show wide range from 0.25 2.50 over narrow potential window (−0.7 −1.1 RHE). In situ attenuated total reflection surface‐enhanced infrared absorption spectroscopy combined density functional theory calculations reveals that synergistic effect between Au Zn sites lowers activation energy barrier molecules facilitates electronic transfer, further highlighting control efficient syngas production using coexisting sites.

Language: Английский

Low‐Coordination Single Au Atoms on Ultrathin ZnIn2S4Nanosheets for Selective Photocatalytic CO2Reduction towards CH4 DOI
Shenghe Si, Hongwei Shou,

Yuyin Mao

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(41)

Published: Aug. 22, 2022

Abstract Selective CO 2 photoreduction to hydrocarbon fuels such as CH 4 is promising and sustainable for carbon‐neutral future. However, lack of proper binding strengths with reaction intermediates makes it still a challenge photocatalytic methanation both high activity selectivity. Here, low‐coordination single Au atoms (Au 1 ‐S ) on ultrathin ZnIn S nanosheets was synthesized by complex‐exchange route, enabling exceptional reduction performance. Under visible light irradiation, /ZnIn catalyst exhibits yield 275 μmol g −1 h selectivity 77 %. As revealed detailed characterizations density functional theory calculations, structure not only display fast carrier transfer underpin its superior activity, but also greatly reduce the energy barrier protonation *CO stabilize *CH 3 intermediate, thereby leading selective generation from photoreduction.

Language: Английский

Citations

166
In-situ constructing Bi@Bi2O2CO3 nanosheet catalyst for ampere-level CO2 electroreduction to formate DOI

Xiao-Du Liang,

Qizheng Zheng,

Nian Wei

et al.

Nano Energy, Journal Year: 2023, Volume and Issue: 114, P. 108638 - 108638

Published: June 25, 2023

Language: Английский

Citations

46
Electronic Structure Design of Transition Metal-Based Catalysts for Electrochemical Carbon Dioxide Reduction DOI Creative Commons
Liang Guo, Jingwen Zhou, Fu Liu

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: 18(14), P. 9823 - 9851

Published: March 28, 2024

With the increasingly serious greenhouse effect, electrochemical carbon dioxide reduction reaction (CO2RR) has garnered widespread attention as it is capable of leveraging renewable energy to convert CO2 into value-added chemicals and fuels. However, performance CO2RR can hardly meet expectations because diverse intermediates complicated processes, necessitating exploitation highly efficient catalysts. In recent years, with advanced characterization technologies theoretical simulations, exploration catalytic mechanisms gradually deepened electronic structure catalysts their interactions intermediates, which serve a bridge facilitate deeper comprehension structure-performance relationships. Transition metal-based (TMCs), extensively applied in CO2RR, demonstrate substantial potential for further modulation, given abundance d electrons. Herein, we discuss representative feasible strategies modulate catalysts, including doping, vacancy, alloying, heterostructure, strain, phase engineering. These approaches profoundly alter inherent properties TMCs interaction thereby greatly affecting rate pathway CO2RR. It believed that rational design modulation fundamentally provide viable directions development toward conversion many other small molecules.

Language: Английский

Citations

34
Stabilizing the oxidation state of catalysts for effective electrochemical carbon dioxide conversion DOI

Zhitong Wang,

Lizhi Xu, Yansong Zhou

et al.

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(12), P. 6295 - 6321

Published: Jan. 1, 2024

Developing sophisticated strategies to stabilize oxidative metal catalysts based on the correlation between dynamic oxidation state and product profile is favorable for efficient electrochemical CO 2 conversion.

Language: Английский

Citations

34
Single-atom tailored atomically-precise nanoclusters for enhanced electrochemical reduction of CO2-to-CO activity DOI Creative Commons

Yi‐Man Wang,

Fang‐Qin Yan, Qian‐You Wang

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Feb. 28, 2024

Abstract The development of facile tailoring approach to adjust the intrinsic activity and stability atomically-precise metal nanoclusters catalysts is great interest but remians challenging. Herein, well-defined Au 8 modified by single-atom sites are rationally synthesized via a co-eletropolymerization strategy, in which uniformly dispersed nanocluster co-entrenched on poly-carbazole matrix. Systematic characterization theoretical modeling reveal that functionalizing single-atoms enable altering electronic structures clusters, amplifies their electrocatalytic reduction CO 2 ~18.07 fold compared isolated clusters. rearrangements structure not only strengthen adsorption key intermediates *COOH, also establish favorable reaction pathway for reaction. Moreover, this strategy fixing cross-linked polymer networks efficiently deduce performance deactivation caused agglomeration during catalytic process. This work contribute explore improvement

Language: Английский

Citations

29
Synergetic catalytic effects by strong metal−support interaction for efficient electrocatalysis DOI Creative Commons
Xue Teng,

Si Di,

Lisong Chen

et al.

eScience, Journal Year: 2024, Volume and Issue: 4(6), P. 100272 - 100272

Published: April 26, 2024

Strong metal−support interaction (SMSI), namely the strong electronic and structural between metal nanoparticles supports, one of most typical synergetic catalytic effects in composite catalysts, has been found critically important design catalyst for thermocatalysis past. Recently, however, great progress SMSI-based made electrocatalysis, such as electrocatalyst electrocatalytic mechanism investigations. To better understand nature effect assisting further development electrocatalysts, a comprehensive in-depth overview highlighting discussing recent advances SMSI electrocatalysis is necessary highly desirable but still absent. Herein, this review firstly presents various strategies designing constructing catalysts featuring SMSI. Further from perspectives characterization techniques towards electron structure, local interfacial morphological features active sites have summarized detail. Importantly, single- bi-functional electrocatalysts effects, key roles during reactions are emphasized. Finally, challenges prospects discussed out-looked to highlight remaining issues future electrocatalysts.

Language: Английский

Citations

28
In-situ reconstruction of active bismuth for enhanced CO2 electroreduction to formate DOI

Chen‐Chen Weng,

Cheng Wang, Yang Song

et al.

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 159732 - 159732

Published: Jan. 1, 2025

Language: Английский

Citations

3
Oxygen vacancy stabilized Bi 2 O 2 CO 3 nanosheet for CO 2 electroreduction at low overpotential enables energy efficient CO‐production of formate DOI Creative Commons
Yangyang Zhang, Yanxu Chen, Rong Liu

et al.

InfoMat, Journal Year: 2022, Volume and Issue: 5(3)

Published: Nov. 2, 2022

Abstract Bismuth‐based electrocatalysts are promising candidates for electrochemical CO 2 reduction to formate attributing the accelerated formation of *OCHO intermediate, while high‐energy consumption remains a major challenge practicability. Herein, we present ultrathin Bi O 3 nanosheets with abundant oxygen vacancy ( Vo ‐BOC‐NS) reconstructed from S, N‐co‐doped bismuth oxides that can act as durable electrocatalyst ‐to‐formate conversion faradic efficiency (FE ) >95%, partial current density 286 mA cm −2 energy 73.8% at −0.62 V (vs. RHE) and low overpotential 200 mV in flow electrolyzer. The theoretical calculations decipher optimize *OCOH adsorption/desorption kinetics. pair‐electrosynthesis tactic co‐production enable superior FE >90% wide cell voltage 2–3.3 total yield rate 3742 μmol h −1 3.3 V, suggesting great potential future industrialization. image

Language: Английский

Citations

54
Weakening the Metal–Support Interactions of M/CeO2 (M = Co, Fe, Ni) Using a NH3-Treated CeO2 Support for an Enhanced Water–Gas Shift Reaction DOI

Xiaochen Sun,

Kun Yuan,

Wang-De Hua

et al.

ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(19), P. 11942 - 11954

Published: Sept. 19, 2022

The metal–support interface plays a crucial role in heterogeneous catalysis. modulation of the interaction (MSI) affords possibility promoting catalytic efficiency per active site. Here, we report strategy to modulate interfacial and then optimize activity Co/CeO2 catalysts for water–gas shift reaction (WGSR) by facile NH3 treatment process CeO2 support. sample Co/800N-CeO2 treated at 800 °C exhibited highest rate 260 μmolCO/(gCo s), which was 23.8 times higher than untreated sample. A combination ex situ characterizations suggested that addition did not only weaken between Co species support strengthen CO adsorption activation ability but also induced oxygen vacancy generation under conditions accelerate H2O activation. Both worked together WGSR via carboxyl pathway low temperature. It worth mentioning N introduced removed after changing catalyst structure conditions. robust 60 h test 400 due coexistence mechanism formate pathways avoiding poisoning effect on sites. construction interfaces could be extended Fe/CeO2 Ni/CeO2 bring great promise design supported wide applications including chemical transformation reactions industrial

Language: Английский

Citations

39
Advanced Catalyst Design and Reactor Configuration Upgrade in Electrochemical Carbon Dioxide Conversion DOI

Zhitong Wang,

Yansong Zhou, Peng Qiu

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(52)

Published: Aug. 20, 2023

Abstract Electrochemical carbon dioxide reduction reaction (CO 2 RR) driven by renewable energy shows great promise in mitigating and potentially reversing the devastating effects of anthropogenic climate change environmental degradation. The simultaneous synthesis energy‐dense chemicals can meet global demand while decoupling emissions from economic growth. However, development CO RR technology faces challenges catalyst discovery device optimization that hinder their industrial implementation. In this contribution, a comprehensive overview current state research is provided, starting with background motivation for technology, followed fundamentals evaluated metrics. Then underlying design principles electrocatalysts are discussed, emphasizing structure–performance correlations advanced electrochemical assembly cells increase selectivity throughput. Finally, review looks to future identifies opportunities innovation mechanism discovery, material screening strategies, assemblies move toward carbon‐neutral society.

Language: Английский

Citations

38