Synergistic Effects of Lewis Acid–Base Pair Sites─Hf-MOFs with Functional Groups as Distinguished Catalysts for the Cycloaddition of Epoxides with CO2 DOI
Lianlian Wang,

Wan‐Zhen Qiao,

Han Liu

et al.

Inorganic Chemistry, Journal Year: 2023, Volume and Issue: 62(9), P. 3817 - 3826

Published: Feb. 23, 2023

The incorporation of Lewis acid–base sites in catalysts has been considered as a significant approach to fabricating bifunctional with efficient catalytic activity for CO2 fixation. In this paper, series Hafnium-based metal–organic frameworks (Hf-MOFs), NU-912(Hf) and NU-912–X(Hf)–X (X = −NH2, −Br, −CN, −I) derivatives assembled by acidic Hf6(μ3–O)4(μ3–OH)4(H2O)4(OH)4 (Hf6) clusters base-attached organic linkers, are successfully synthesized facile ligand functionalization method. These isostructural Hf-MOFs, which exhibit diamond channels 1.3 nm diameter, great chemical stability, adsorption capacity, have evaluated the cycloaddition reaction epoxides. Catalytic experiments reveal that micropore environments these MOFs an outstanding impact on activity. Remarkably, NU-912(Hf)–I serves heterogeneous catalyst under mild conditions due high density acid Hf6 cluster centers strong base functional groups, surpassing most reported MOF-based catalysts.

Language: Английский

Attenuating metal-substrate conjugation in atomically dispersed nickel catalysts for electroreduction of CO2 to CO DOI Creative Commons
Qiyou Wang, Kang Liu,

Kangman Hu

et al.

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: Oct. 14, 2022

Atomically dispersed transition metals on carbon-based aromatic substrates are an emerging class of electrocatalysts for the electroreduction CO

Language: Английский

Citations

143
Vertical Cu Nanoneedle Arrays Enhance the Local Electric Field Promoting C2 Hydrocarbons in the CO2 Electroreduction DOI

Yajiao Zhou,

Yanqing Liang,

Junwei Fu

et al.

Nano Letters, Journal Year: 2022, Volume and Issue: 22(5), P. 1963 - 1970

Published: Feb. 15, 2022

Electrocatalytic reduction of CO2 to multicarbon products is a potential strategy solve the energy crisis while achieving carbon neutrality. To improve efficiency in Cu-based catalysts, optimizing *CO adsorption and reducing barrier for carbon-carbon (C-C) coupling are essential features. In this work, strong local electric field obtained by regulating arrangement Cu nanoneedle arrays (CuNNAs). performance tests indicate that an ordered array reaches 59% Faraday (FEC2) at -1.2 V (vs RHE), compared FEC2 20% disordered (CuNNs). As such, very high fields achieved leads accumulation K+ ions, which benefit both C-C coupling. Our results contribute design highly efficient catalysts products.

Language: Английский

Citations

140
Electrocatalytic CO2 Reduction to C2+ Products in Flow Cells DOI
Qin Chen, Xiqing Wang,

Yajiao Zhou

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(5)

Published: Aug. 31, 2023

Abstract Electrocatalytic CO 2 reduction into value‐added fuels and chemicals by renewable electric energy is one of the important strategies to address global shortage carbon emission. Though classical H‐type electrolytic cell can quickly screen high‐efficiency catalysts, low current density limited mass transfer process essentially impede its industrial applications. The cells based on electrolyte flow system (flow cells) have shown great potential for devices, due higher density, improved local concentration, better efficiency. design optimization are significance further accelerate industrialization electrocatalytic reaction (CO RR). In this review, progress RR C 2+ products concerned. Firstly, main events in development outlined. Second, principles products, architectures, types summarized. Third, optimizing generate reviewed detail, including cathode, anode, ion exchange membrane, electrolyte. Finally, preliminary attempts, challenges, research prospects toward discussed.

Language: Английский

Citations

89
Ordered Ag Nanoneedle Arrays with Enhanced Electrocatalytic CO2 Reduction via Structure-Induced Inhibition of Hydrogen Evolution DOI
Qin Chen, Kang Liu,

Yajiao Zhou

et al.

Nano Letters, Journal Year: 2022, Volume and Issue: 22(15), P. 6276 - 6284

Published: Aug. 1, 2022

Silver is an attractive catalyst for converting CO2 into CO. However, the high activation barrier and hydrogen evolution side reaction seriously limit its practical application industrial perspective. Here, ordered Ag nanoneedle array (Ag-NNAs) was prepared by template-assisted vacuum thermal-evaporation electroreduction The structure induces a strong local electric field at tips, which not only reduces but also increases energy (HER). Moreover, endows surface hydrophobicity, can regulate adsorption of water molecules interface thus dynamically inhibit competitive HER. As result, optimal Ag-NNAs exhibits 91.4% Faradaic efficiency (FE) CO over 700 min −1.0 V vs RHE. This work provides new concept structures in electrocatalytic reduction reactions.

Language: Английский

Citations

84
Borate narrowed band gap of nickel-iron layer double hydroxide to mediate rapid reconstruction kinetics for water oxidation DOI

Hanxiao Liao,

Ganghai Ni,

Pengfei Tan

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 317, P. 121713 - 121713

Published: July 5, 2022

Language: Английский

Citations

82
Stimulate the hidden catalysis potential and exposure of nickel site in NiSe@CNTs result in ultra-high HER/OER activity and stability DOI
Hongyao Xue, Tongqing Yang, Ziming Zhang

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 330, P. 122641 - 122641

Published: March 15, 2023

Language: Английский

Citations

80
Heteroatoms Induce Localization of the Electric Field and Promote a Wide Potential‐Window Selectivity Towards CO in the CO2 Electroreduction DOI Creative Commons
Chao Cai, Bao Liu, Kang Liu

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(44)

Published: Sept. 8, 2022

Carbon dioxide electroreduction (CO2 RR) is a sustainable way of producing carbon-neutral fuels. Product selectivity in CO2 RR regulated by the adsorption energy reaction-intermediates. Here, we employ differential phase contrast-scanning transmission electron microscopy (DPC-STEM) to demonstrate that Sn heteroatoms on Ag catalyst generate very strong and atomically localized electric fields. In situ attenuated total reflection infrared spectroscopy (ATR-IR) results verified field enhances *COOH, thus favoring production CO during RR. The Ag/Sn exhibits an approximately 100 % at wide range potentials (from -0.5 -1.1 V, versus reversible hydrogen electrode), with remarkably high efficiency (EE) 76.1 %.

Language: Английский

Citations

75
How to select heterogeneous CO 2 reduction electrocatalyst DOI Creative Commons

Ji Shen,

Dingsheng Wang

Deleted Journal, Journal Year: 2023, Volume and Issue: 3, P. e9120096 - e9120096

Published: Sept. 1, 2023

As an important part of carbon neutralization, dioxide electroreduction reaction (CO2RR) can convert CO2 into high value-added chemicals and fuels to realize the recycling resources solve problem environmental pollution. Therefore, exploring element species surface structure catalyst plays a central role in improving performance catalyst, enhancing conversion efficiency forming C1 C2+ products. Here, we summarize recent progress selective regulation CO2RR products by different elements. In particular, emphasize structure-property relationship microenvironment metal center substrate, heteroatom doping, hydrogen bond network metal-free polymer, construction heterogeneous catalytic system. At same time, advances for identification active sites mechanistic studies on process reducing are reviewed, as well comprehensive review final Finally, outline inevitable challenges faced present our own recommendations aimed at contributing resource utilization.

Language: Английский

Citations

53
Regulating the Electronic Configuration of Ni Sites by Breaking Symmetry of Ni‐Porphyrin to Facilitate CO2 Photocatalytic Reduction DOI
Yuan‐Hui Zhong, Yang Wang,

Sheng‐Yi Zhao

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(25)

Published: Feb. 10, 2024

Abstract Adapting the coordination environment to influence electronic configuration of active sites represents an efficient approach for improving photocatalytic performance CO 2 reduction reaction (CO RR) but how execute it precisely remains challenging. Herein, heteroatom‐substitution in Ni‐porphyrin break symmetry Ni center is proposed be effective solution. Based on this, two symmetry‐breaking Ni‐porphyrins, namely Ni(Cl)ON 3 Por and Ni(Cl)SN , are designed successfully prepared. By theoretical calculation, found that efficiently regulates d orbital energy levels center. Furthermore, experimental findings jointly revealed Ni‐porphyrins facilitates generation highly reactive I species during catalytic process, effectively stabilizing reducing barrier formation key * COOH intermediate. As a result, gave production rates 24.7 38.8 mmol g −1 h as well selectivity toward 94.0% 96.4%, respectively, outperforming symmetric NiN 4 rate 6.6 82.8%). These offer microscopic insights into modulate activity by tuning rational design competent catalyst RR photocatalysis.

Language: Английский

Citations

23
Electrocatalytic C–N coupling for urea synthesis: a critical review DOI

Chuanju Yang,

Zhe Li, Junpeng Xu

et al.

Green Chemistry, Journal Year: 2024, Volume and Issue: 26(9), P. 4908 - 4933

Published: Jan. 1, 2024

Strategies for building efficient electrocatalytic urea synthesis systems.

Language: Английский

Citations

19