Construction of Low‐Coordination Cu−C2 Single‐Atoms Electrocatalyst Facilitating the Efficient Electrochemical CO2 Reduction to Methane DOI
Peng Zhao, Hao Jiang,

Haidong Shen

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(49)

Published: Oct. 25, 2023

Constructing Cu single-atoms (SAs) catalysts is considered as one of the most effective strategies to enhance performance electrochemical reduction CO2 (e-CO2 RR) towards CH4 , however there are challenges with activity, selectivity, and a cumbersome fabrication process. Herein, by virtue meta-position structure alkynyl in 1,3,5-triethynylbenzene interaction between -C≡C-, SAs electrocatalyst (Cu-SAs/HGDY), containing low-coordination Cu-C2 active sites, was synthesized through simple efficient one-step method. Notably, this represents first achievement preparing coordination structure, which exhibited high -to-CH4 selectivity (72.1 %) partial current density 230.7 mA cm-2 turnover frequency 2756 h-1 dramatically outperforming currently reported catalysts. Comprehensive experiments calculations verified not only endowed center more positive electricity but also promoted formation H•, contributed outstanding e-CO2 RR electrocatalytic Cu-SAs/HGDY. Our work provides novel H⋅-transferring mechanism for offers protocol preparation two-coordinated

Language: Английский

Two-Dimensional Carbon Graphdiyne: Advances in Fundamental and Application Research DOI

Xuchen Zheng,

Siao Chen,

Jinze Li

et al.

ACS Nano, Journal Year: 2023, Volume and Issue: 17(15), P. 14309 - 14346

Published: July 20, 2023

Graphdiyne (GDY), a rising star of carbon allotropes, features two-dimensional all-carbon network with the cohybridization sp and sp2 atoms represents trend research direction in development materials. The sp/sp2-hybridized structure GDY endows it numerous advantages advancements controlled growth, assembly, performance tuning, many studies have shown that has been key material for innovation fields catalysis, energy, photoelectric conversion, mode conversion transformation electronic devices, detectors, life sciences, etc. In past ten years, fundamental scientific issues related to understood, showing differences from traditional materials chemical physical properties mechanisms, attracting extensive attention scientists. gradually developed into one frontiers chemistry science, entered rapid period, producing large numbers applied achievements For exploration frontier concepts phenomena science research, there is great potential promote progress intelligent information, optoelectronics, sciences. this review, self-assembly method, aggregation structure, modification, doping are shown, theoretical calculation simulation also fully introduced. particular, applications its formed aggregates energy storage, photoelectronic, biomedicine, environmental separation

Language: Английский

Citations

147
Recent Advances on Single‐Atom Catalysts for CO2 Reduction DOI Creative Commons

Lizhen Liu,

Mingtao Li, Fang Chen

et al.

Small Structures, Journal Year: 2022, Volume and Issue: 4(3)

Published: Oct. 27, 2022

Continuous consumption of fossil energy and excessive CO 2 emission severely restrict human society. Sustainable carbon cycle is a promising technology to simultaneously relieve greenhouse effect crisis based on electrocatalysis photocatalysis. However, the conversion efficiency confined by poor carriers utilization insufficient reactive sites. Single‐atom catalysts (SACs) display outstanding performance in effectively overcoming aforementioned problems. Herein, recent advances SACs for enhancing efficiency, selectivity, long‐range stability reduction are provided. First, characteristics have been introduced detail provide rational design relationship between structure performance, including type, structure, synthesis SACs. Then, high electrocatalytic, photocatalytic, thermocatalytic has discussed disclosing reaction mechanism, such as charge transfer, activation barriers, pathway. In particular, strategies summarized deep insight into designing developing more efficient Finally, an outlook current challenges perspectives proposed. This review aims systematic reference advanced catalytic conversion.

Language: Английский

Citations

94
Graphynes and Graphdiynes for Energy Storage and Catalytic Utilization: Theoretical Insights into Recent Advances DOI
Hao Li,

Jong Hyeon Lim,

Yipin Lv

et al.

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(8), P. 4795 - 4854

Published: March 15, 2023

Carbon allotropes have contributed to all aspects of people's lives throughout human history. As emerging carbon-based low-dimensional materials, graphyne family members (GYF), represented by graphdiyne, a wide range potential applications due their superior physical and chemical properties. In particular, graphdiyne (GDY), as the leader family, has been practically applied various research fields since it was first successfully synthesized. GYF large surface area, both sp sp2 hybridization, certain band gap, which considered originate from overlap carbon 2pz orbitals inhomogeneous π-bonds atoms in different hybridization forms. These properties mean GYF-based materials still many be developed, especially energy storage catalytic utilization. Since most yet synthesized not developed for long time, theoretical results application should shared experimentalists attract more intentions. this Review, we summarized discussed synthesis, structural properties, insights, hoping provide viewpoints comments.

Language: Английский

Citations

82
Review on strategies for improving the added value and expanding the scope of CO2 electroreduction products DOI
Minghang Jiang, Huaizhu Wang, Mengfei Zhu

et al.

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(10), P. 5149 - 5189

Published: Jan. 1, 2024

This review summarizes promising strategies including the design of catalysts and construction coupled electrocatalytic reaction systems, aimed at achieving selective production various products from CO 2 electroreduction.

Language: Английский

Citations

75
Emerging Xene‐Based Single‐Atom Catalysts: Theory, Synthesis, and Catalytic Applications DOI
Mengke Wang, Yi Hu,

Junmei Pu

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(3)

Published: June 17, 2023

Abstract In recent years, the emergence of novel 2D monoelemental materials (Xenes), e.g., graphdiyne, borophene, phosphorene, antimonene, bismuthene, and stanene, has exhibited unprecedented potentials for their versatile applications as well addressing new discoveries in fundamental science. Owing to unique physicochemical, optical, electronic properties, emerging Xenes have been regarded promising candidates community single‐atom catalysts (SACs) active sites or support matrixes significant improvement intrinsic activity selectivity. order comprehensively understand relationships between structure property Xene‐based SACs, this review represents a comprehensive summary from theoretical predictions experimental investigations. Firstly, calculations regarding both anchoring on doping/substituting heteroatoms at are briefly summarized. Secondly, controlled synthesis precise characterization presented SACs. Finally, current challenges future opportunities development SACs highlighted.

Language: Английский

Citations

62
In Situ Carbon-Encapsulated Copper-Doped Cerium Oxide Derived from MOFs for Boosting CO2-to-CH4 Electro-Conversion DOI
Ya Zhang, Xiaoyu Zhang, Wei‐Yin Sun

et al.

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(2), P. 1545 - 1553

Published: Jan. 10, 2023

Electrochemical CO2 reduction reaction offers enormous potential for achieving carbon neutrality by converting back into value-added chemicals and fuels. In the quest to resolve its current problem of poor selectivity or low density toward one specific product, we propose a feasible strategy develop carbon-encapsulated copper-doped cerium oxide composite (Cu/CeO2@C) one-pot pyrolysis metal–organic framework (MOF) precursors. The optimal Cu/CeO2@C achieves high CH4 Faraday efficiency 80.3% large partial 138.6 mA cm–2. We demonstrate that enhanced activity is attributed synergistic effect Cu/CeO2 in situ-formed with robust channels assist charge transfer. Operando attenuated total reflection–infrared spectroscopic characterization reveals can strengthen adsorption intermediates on active sites, facilitating kinetics ultimately improving CH4.

Language: Английский

Citations

58
Graphdiyne‐Based Single‐Atom Catalysts with Different Coordination Environments DOI
Xinliang Fu,

Xin Zhao,

Tong‐Bu Lu

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(16)

Published: Feb. 1, 2023

Abstract As a special carbon material, graphdiyne (GDY) features the superiorities of incomplete charge transfer effect on atomic level, tunable electronic structure and anchoring metal atoms directly with organometallic coordination bonds M (metal)‐C (alkynyl in GDY), providing it an ideal platform to construct single‐atom catalysts (ACs). The environment single anchored GDY plays key role their catalytic performance. mini‐review highlights state‐of‐the‐art progress rational design GDY‐based ACs applications, mainly reveals relationship between engineering corresponding Finally, some prospects concerning future development energy conversion are also discussed.

Language: Английский

Citations

57
Constructing matched active sites for robust photocatalytic dry reforming of methane DOI Creative Commons

Chengxuan He,

Shiqun Wu, Qixin Li

et al.

Chem, Journal Year: 2023, Volume and Issue: 9(11), P. 3224 - 3244

Published: July 25, 2023

Language: Английский

Citations

51
Porous Organic Polymers‐Based Single‐Atom Catalysts for Sustainable Energy‐Related Electrocatalysis DOI
Haoyang Li, Fuping Pan, Qin Chen

et al.

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(28)

Published: June 8, 2023

Abstract Single‐atom catalysts (SACs) have been emerging as attractive catalytic materials in electrocatalysis for sustainable energy storage and conversion. To realize the practical implementation of SACs, reliable support is highly imperative to stabilize atomically dispersed metals with strong metal–support interaction, tunable local electronic environment, favorable electron/mass transport. Thanks great designability tunability composition, structure, morphology, porous organic polymers (POPs) demonstrated grand promise appropriate platforms toward design SACs at molecular level fabrication a controlled manner. Herein, comprehensive overview recent advances elucidation general principles, effective synthesis approaches, fundamental mechanisms boosting development high‐performance POPs‐based electrocatalytic transformations provided. The authors first outline rationales using supports principles electrocatalysis, followed by discussing approaches utilizing POPs POPs‐derived nanocarbons host single‐atom metals. Then, state‐of‐the‐art their applications heterogeneous (ORR, OER, HER, CO 2 RR, NRR) are discussed, which focus on revealing structure–performance correlation mechanisms. Finally, challenges strategies associated rational suggested.

Language: Английский

Citations

47
Achievements and challenges of copper‐based single‐atom catalysts for the reduction of carbon dioxide to C2+ products DOI Creative Commons

Tianmi Tang,

Zhenlü Wang, Jingqi Guan

et al.

Exploration, Journal Year: 2023, Volume and Issue: 3(5)

Published: July 26, 2023

Copper is the only metal that can convert CO

Language: Английский

Citations

45