Adjacent Metal Atomic Pairs Within Atomically Dispersed Catalysts for Reaching a Synergistic Electrocatalytic CO2 Reduction: A Review DOI
Changli Wang,

Zunhang Lv,

Xiao Feng

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(21)

Published: Feb. 27, 2024

Abstract In response to the global climate change and energy crisis, electrocatalytic CO 2 reduction reaction (ECR) is regarded as one of potential ways simultaneously reach conversion obtain various value‐added products. Currently, several challenges remain for in‐depth understanding ECR from fundamentals, including ambiguous structure‐activity relationships, uncontrollable catalytic selectivity, complex mechanisms. Compared traditional metal nanoparticle‐based materials, atomically dispersed catalysts (ADCs) have aroused significant interest owing their maximal atomic utilization simplified site configuration, offering a superior platform discussing relationships during ECR. Especially, adjacent pairs (AAPs) within ADCs are gradually emphasized novel concept follow synergistic mechanisms Herein, first time broad AAPs analyzed how reached effect summarized. view varying on different supports, three types supports illustrated (containing graphene model, functional porous frameworks, metals oxides), aiming help scholars with more insights in broadening feasible ADCs.

Language: Английский

Recent advances in metal–organic framework-derived materials for electrocatalytic and photocatalytic CO2 reduction DOI

Yu‐Tao Zheng,

Shumin Li, Ning‐Yu Huang

et al.

Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 510, P. 215858 - 215858

Published: April 15, 2024

Language: Английский

Citations

31
Covalent Organic Frameworks for Photocatalytic Hydrogen Peroxide Generation DOI

Akhtar Alam,

Bidhan Kumbhakar,

Avanti Chakraborty

et al.

ACS Materials Letters, Journal Year: 2024, Volume and Issue: 6(5), P. 2007 - 2049

Published: April 17, 2024

Hydrogen peroxide (H2O2), a valuable chemical, is widely used as powerful oxidizing agent in chemical synthesis, pharmaceuticals, medical disinfection, and environmental treatment industries. Currently, over 95% of H2O2 produced industrially using the anthraquinone process, which associated with its high energy consumption hazardous byproducts. Therefore, photochemical synthesis from water oxygen covalent organic framework based photocatalysts have attracted considerable attention. This review aims to outline recent achievements, challenges future prospects COFs heterogeneous for sustainable generation. We summarize chronological development COFs, different mechanisms involved, detailed experiments quantification methods photocatalytic The puts forward an outlook, highlighting advantages limitations anticipate that this will provide insight into current progress inspire next-generation production.

Language: Английский

Citations

26
Downsizing Porphyrin Covalent Organic Framework Particles Using Protected Precursors for Electrocatalytic CO2 Reduction DOI Creative Commons
Kenichi Endo, Asif Hassan Raza, Liang Yao

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(19)

Published: Feb. 1, 2024

Abstract Covalent organic frameworks (COFs) are promising electrocatalyst platforms owing to their designability, porosity, and stability. Recently, COFs with various chemical structures developed as efficient electrochemical CO 2 reduction catalysts. However, controlling the morphology of COF catalysts remains a challenge, which can limit electrocatalytic performance. Especially, while porphyrin show catalytic properties, particle size is mostly large uncontrolled because severe aggregation crystallites. In this work, new synthetic methodology for rationally downsized catalyst particles reported, where tritylated amine employed novel protected precursor synthesis. Trityl protection provides high solubility precursor, its deprotection proceeds in situ under typical synthesis conditions. Subsequent homogeneous nucleation colloidal growth yield smaller than conventional synthesis, suppressed crystallite aggregation. The exhibit superior performance reduction, higher production rate faradaic efficiency compared particles. improved attributed contact area conductive agent. This study reveals an important factor evaluation electrocatalysts strategy control it.

Language: Английский

Citations

24
Macrocycle-embedded metal-covalent organic frameworks for catalysis: A bridge between covalent and non-covalent functional frameworks DOI
Menghao Li,

Changling Xu,

Ying‐Wei Yang

et al.

Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 512, P. 215894 - 215894

Published: April 26, 2024

Language: Английский

Citations

24
Elaborate Modulating Binding Strength of Intermediates via Three‐component Covalent Organic Frameworks for CO2 Reduction Reaction DOI
Minghao Liu, Cheng‐Xing Cui, Shuai Yang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(20)

Published: Feb. 26, 2024

Abstract The catalytic performance for electrocatalytic CO 2 reduction reaction (CO RR) depends on the binding strength of reactants and intermediates. Covalent organic frameworks (COFs) have been adopted to catalyze RR, their abilities are tuned via constructing donor‐acceptor (DA) systems. However, most DA COFs single donor acceptor units, which caused wide‐range but lacking accuracy in modulating More elaborate regulation interactions with intermediates necessary challenge construct high‐efficiency catalysts. Herein, three‐component COF D‐A‐A units was first constructed by introducing electron‐rich diarylamine unit, electron‐deficient benzothiazole Co‐porphyrin units. Compared two‐component COFs, designed exhibit elevated electronic conductivity, enhanced reducibility, high efficiency charge transfer, further improving RR faradic 97.2 % at −0.8 V activity partial current density 27.85 mA cm −2 −1.0 exceed other COFs. Theoretical calculations demonstrate that sites suitable ability intermediates, benefit formation *COOH desorption *CO. This work offers valuable insights advancement multi‐component enabling modulated transfer improve activity.

Language: Английский

Citations

22
Ionic Covalent Organic Frameworks in Adsorption and Catalysis DOI
Minghao Liu, Qing Xu, Gaofeng Zeng

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(22)

Published: April 2, 2024

Abstract The ion extraction and electro/photo catalysis are promising methods to address environmental energy issues. Covalent organic frameworks (COFs) a class of template construct absorbents catalysts because their stable frameworks, high surface areas, controllable pore environments, well‐defined catalytic sites. Among them, ionic COFs as unique crystalline porous materials, with charges in the or along walls, have shown different properties resulting performance these applications those from charge‐neutral COFs. In this review, current research progress based on for conversion, including cationic/anionic materials is reviewed terms synthesis strategy, modification methods, mechanisms adsorption catalysis, well applications. Finally, we demonstrated challenges future development design strategies

Language: Английский

Citations

18
Covalent-Metal organic Frameworks: Preparation and applications DOI
Zhaobo Wang, Chen Wang, Qiming Hu

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 483, P. 149217 - 149217

Published: Feb. 2, 2024

Language: Английский

Citations

17
Atomistic Structural Engineering of Conjugated Microporous Polymers Promotes Photocatalytic Biomass Valorization DOI
Yuchen Yan, Xiaohan Yu,

Chaochen Shao

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(42)

Published: June 9, 2023

Abstract Polymer photocatalysts have great promise for solar fuel production due to their flexible structural and functional designability. However, photocatalytic efficiencies are still unsatisfactory, limited by intrinsically large exciton binding energy fast charge recombination. Herein, the atomistic engineering of donor–acceptor (D−A) polymer enhanced separation hydrogen is proposed. By changing electron affinity acceptor units, delocalization polymeric networks can be readily tuned, resulting in efficiency activity. The optimal sample shows highest H 2 rate 3207 µmol g −1 h presence ascorbic acid as sacrificial agent. Moreover, coupled with almost stoichiometrical conversion 5‐hydroxymethyl furfural 2,5‐diformylfuran.

Language: Английский

Citations

40
Simultaneous Capture of CO2 Boosting Its Electroreduction in the Micropores of a Metal–organic Framework DOI
Yuanyuan Liu, Jia‐Run Huang, Haolin Zhu

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(52)

Published: Oct. 2, 2023

Integration of CO2 capture capability from simulated flue gas and electrochemical reduction reaction (eCO2 RR) active sites into a catalyst is promising cost-effective strategy for carbon neutrality, but great difficulty. Herein, combining the mixed breakthrough experiments eCO2 RR tests, we showed that an Ag12 cluster-based metal-organic framework (1-NH2 , aka bpy-NH2 ), simultaneously possessing as "CO2 relays" sites, can not only utilize its micropores to efficiently (CO2 : N2 =15 85, at 298 K), also catalyze adsorbed CO with ultra-high conversion 60 %. More importantly, performance (a Faradaic efficiency (CO) 96 % commercial current density 120 mA cm-2 very low cell voltage -2.3 V 300 hours full-cell energy 56 %) under atmosphere close 100 atmosphere, higher than those all reported catalysts potentials atmosphere. This work bridges gap between enrichment/capture RR.

Language: Английский

Citations

34
Highly Enhancing CO2 Photoreduction by Metallization of an Imidazole‐linked Robust Covalent Organic Framework DOI
Tian‐Xiang Luan, Jiarui Wang, Keyu Li

et al.

Small, Journal Year: 2023, Volume and Issue: 19(44)

Published: June 30, 2023

Converting CO2 into value-added chemicals to solve the issues caused by carbon emission is promising but challenging. Herein, embedding metal ions (Co2+ , Ni2+ Cu2+ and Zn2+ ) an imidazole-linked robust photosensitive covalent organic framework (PyPor-COF), effective photocatalysts for conversion are rationally designed constructed. Characterizations display that all of metallized PyPor-COFs (M-PyPor-COFs) remarkably high enhancement in their photochemical properties. Photocatalysis reactions reveal Co-metallized PyPor-COF (Co-PyPor-COF) achieves a CO production rate as up 9645 µmol g-1 h-1 with selectivity 96.7% under light irradiation, which more than 45 times higher metal-free PyPor-COF, while Ni-metallized (Ni-PyPor-COF) can further tandem catalyze generated CH4 463.2 . Experimental analyses theory calculations remarkable performance on photoreduction should be attributed incorporated sites COF skeleton, promotes adsorption activation desorption even reduces reaction energy barrier formation different intermediates. This work demonstrates metallizing photoactive COFs, achieved.

Language: Английский

Citations

32