Two-Dimensional Kagome Covalent Organic Frameworks with Single Atomic Co Sites for Superior Photocatalytic CO2 Reduction DOI
Yuhui Wang, Tingting Sun, Tianyu Zheng

et al.

ACS Materials Letters, Journal Year: 2023, Volume and Issue: 6(1), P. 140 - 152

Published: Dec. 7, 2023

Covalent organic frameworks (COFs) have attracted great attention as pivotal photocatalysts for efficient CO2 photoreduction into value-added fuels, which hold promise simultaneously mitigating global warming and the energy crisis. However, synthesis of COFs with a high crystalline state hierarchically porous structure to boost is still an enormous challenge rarely reported, probably because dependence upon monomers rigorous preparation conditions. Herein, series functional kagome (kg m) topologic 2D crystallinity porosity were synthesized based on condensation 4,4′,4″,4‴-(ethene-1,1,2,2-tetrayl)tetraaniline (ETTA) 2,2′-bipyridyl-5,5′-dialdehyde (Bpy-CHO) building units combined postmodification strategy, named ETTA-Bpy-COF-M (M = H, Fe, Co, Ni, or Cu). Stimulated by unique kg m topologized framework well-ordered hierarchical micropores mesopores, abundant exposed atomic Co sites, remarkable photoelectrical performance, ETTA-Bpy-COF-Co used photocatalyst catalyzing CO2-to-CO photoconversion exhibits CO yield rate (9398.14 μmol g–1 h–1), large selectivity (92.73%), good durability. Experimental theoretical analyses demonstrated that superior performance catalyzed was attributed desirable cooperative contribution topological hexagonal triangular pores well active can promote photoexcited charge carrier kinetics, enhance adsorption activation, reduce barriers *COOH generation desorption. This work opens new way COF photosynthesis reduction offers precious insights related studies in future.

Language: Английский

Defect and nanostructure engineering of polymeric carbon nitride for visible-light-driven CO2 reduction DOI

Ziruo Zhou,

Wenyu Guo,

Tingyu Yang

et al.

Chinese Journal of Structural Chemistry, Journal Year: 2024, Volume and Issue: 43(3), P. 100245 - 100245

Published: Feb. 5, 2024

Language: Английский

Citations

69
Structural Motifs in Covalent Organic Frameworks for Photocatalysis DOI

Liyang Qin,

Chengdi Ma,

Jian Zhang

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: March 10, 2024

Abstract Covalent organic frameworks (COFs) attract significant attention due to their ordered, crystalline, porous, metal‐free, and predictable structures. These unique characteristics offer great opportunities for the diffusion transmission of photogenerated charges during photocatalysis. Currently, a considerable number COFs are used as metal‐free semiconductor photocatalysts. This review aims understand relationships between structure photocatalysis performance provides in‐depth insight into synthetic strategy improve performance. Subsequently, focuses on structural motif in sustainable photocatalytic hydrogen evolution, carbon dioxide reduction, peroxide generation, compound transformations. Last, conjunction with progress achieved challenges yet be overcome, candid discussion is undertaken regarding field COF photocatalysis, accompanied by presentation potential research avenues future directions. seeks provide readers comprehensive understanding pivotal role robust guidance innovative utilization

Language: Английский

Citations

61
Stepwise Protonation of Three‐Dimensional Covalent Organic Frameworks for Enhancing Hydrogen Peroxide Photosynthesis DOI

Pengfei Dong,

Xinyu Xu,

Taikang Wu

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(30)

Published: May 13, 2024

Abstract Three‐dimensional covalent organic frameworks (3D COFs), recognized for their tailorable structures and accessible active sites, offer a promising platform developing advanced photocatalysts. However, the difficulty in synthesis functionalization of 3D COFs hinders further development. In this study, we present series 3D‐ bcu ‐COFs with 8 connected porphyrin units linked by linear linkers through imine bonds as versatile photocatalyst design. The photoresponse was initially modulated functionalizing benzo‐thiadiazole or benzo‐selenadiazole groups. Furthermore, taking advantage well‐exposed sites ‐COFs, photocatalytic activity optimized stepwise protonation centers. dual protonated COF groups exhibited enhanced charge separation, leading to an increased H 2 O production under visible light. This enhancement demonstrates combined benefits linker on efficiency.

Language: Английский

Citations

24
12 Connecting Sites Linked Three‐dimensional Covalent Organic Frameworks with Intrinsic Non‐interpenetrated shp Topology for Photocatalytic H2O2 Synthesis DOI
Xinxin Wang, Yucheng Jin, Ning Li

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(15)

Published: Feb. 9, 2024

Developing high connectivity (>8) three-dimensional (3D) covalent organic frameworks (COFs) towards new topologies and functions remains a great challenge owing to the difficulty in getting building blocks. This however represents most important step promoting diversity of COFs due still limited dynamic bonds available for constructing at this stage. Herein, highly connected phthalocyanine-based (Pc-based) 3D MPc-THHI-COFs (M=H

Language: Английский

Citations

22
Rational Design of 3D Space Connected Donor–Acceptor System in Covalent Organic Frameworks for Enhanced Photocatalytic Performance DOI

Yinghui Xie,

Fengyi Mao,

Qiuyu Rong

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(52)

Published: Aug. 27, 2024

Abstract Herein, a rational strategy is presented to reduce the energy barrier of singlet ground state excited transitions, whilst simultaneously reducing losses in populating triplet states. The approach relies on constructing 3D space connected donor–acceptor systems COFs. D–A system 8‐connected COFs (denoted as COF‐1 and COF‐2) allows efficient transfer electrons, overcoming traditional electron transport limitations 2D significantly boosting solar utilization efficiency under visible light irradiation. COF‐2, possessing an extended π‐conjugated structure relative COF‐1, demonstrated high selectivity for photocatalytic generation H 2 O (6.93 mmol g −1 h ) natural seawater without need sacrificial reagents, exceeding performance most previously reported COF‐based photocatalysts. this work offers new optimizing photocatalysts production other applications.

Language: Английский

Citations

19
Progress of Covalent Organic Framework Photocatalysts: From Crystallinity–Stability Dilemma to Photocatalytic Performance Improvement DOI

Huili Ran,

Quanlong Xu, Yun Yang

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(15), P. 11675 - 11704

Published: July 22, 2024

Language: Английский

Citations

17
Covalent Organic Frameworks (COFs) for CO2 Utilizations DOI Creative Commons

Maha H. Alenazi,

Aasif Helal, Mohd Yusuf Khan

et al.

Carbon Capture Science & Technology, Journal Year: 2025, Volume and Issue: unknown, P. 100365 - 100365

Published: Jan. 1, 2025

Language: Английский

Citations

6
Hetero-Motif Molecular Junction Photocatalysts: A New Frontier in Artificial Photosynthesis DOI
Lei Zhang, Jiang Liu, Ya‐Qian Lan

et al.

Accounts of Chemical Research, Journal Year: 2024, Volume and Issue: 57(6), P. 870 - 883

Published: Feb. 29, 2024

ConspectusTo cope with the increasingly global greenhouse effect and energy shortage, it is urgent to develop a feasible means convert anthropogenic excess carbon dioxide (CO2) into resources. The photocatalytic CO2 reduction reaction (CO2RR) coupled water oxidation (WOR), known as artificial photosynthesis, green, clean, promoting strategy deal above issues. Among reported systems for reduction, main challenge achieve WOR simultaneously due limited charge separation efficiency complicated dynamic process. To address problem, scientists have assembled two nanosemiconductor motifs CO2RR heterojunction photocatalyst realize photosynthesis. However, difficult clearly explore corresponding catalytic mechanism establish an accurate structure–activity relationship at molecular level their aperiodic distribution structural information. Standing on shoulders of photocatalysts, new-generation material, hetero-motif junction (HMMJ) has been developed studied by our laboratory. A class crystalline materials well-defined periodic structure, adjustable assembly mode, semiconductor-like properties, which composed predesigned respectively, coordination or covalent bonds. intrinsic properties make these catalysts susceptible functional modifications improve light absorption electrical conductivity. small size short distance can greatly promote photogenerated electron–hole migration. Based advantages, they be used potential excellent photocatalysts Notably, explicit information determined single-crystal powder X-ray diffraction provide visual platform mechanism. More importantly, connection number, spatial distance, interaction, arrangement mode well-designed detailed that hardly in nanoheterojunction systems. In this regard, HMMJ new frontier photosynthesis serve important bridge between solid photocatalysts. Thus, very summarize state-of-the-art give in-depth insight future development.In Account, we summarized recent advances using mainly focusing results lab. We present overview current knowledge about introduce design schemes unique advantages compared other construction strategies application explain why junctions promising show powerful studying photocatalysis. dynamics are illustrated. Finally, bring outlook challenges development prospects believe Account will afford insights high-efficiency guidance more atom-economic, environmentally friendly, sustainable way.

Language: Английский

Citations

15
A General Base-free Route toward the Building of Metal N-Heterocyclic Carbenes into Covalent Organic Frameworks for CO2 Conversion DOI
Chang He, Duan‐Hui Si, Lili Han

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(6), P. 3943 - 3954

Published: Feb. 27, 2024

Covalent organic frameworks (COFs) would be a promising platform to immobilize metal N-heterocyclic carbenes (M-NHCs) for efficient CO2 conversion, but they are seldom reported. Herein, we develop facile base-free strategy prepare M-NHCs (M = Ir, Au, Pd) decorated M-NHC–COFs (Ir-NHC–COF, Au-NHC–COF, and Pd-NHC–COF) via the reactions of imidazolium carboxylate functionalized NHC-based COF (NHC–CO2–COF) with corresponding complexes under mild conditions. This synthesis method generation desired M-NHC single sites avoids handling free use strong bases. The obtained Ir-NHC–COF catalyst showed catalytic activity recyclability in hydrogenation process, attaining noteworthy turnover frequency up 17244 h–1, which placed it among top-performing heterogeneous catalysts this reaction. study presents universal straightforward approach attaching functional onto COFs, offering combined advantages acting as highly reactions. general widely applicable other M-NHC-functionalized porous materials covalently bound various applications future.

Language: Английский

Citations

14
Synthetic Leaves Based on Crystalline Olefin-Linked Covalent Organic Frameworks for Efficient CO2 Photoreduction with Water DOI
Na Yang,

Wenkai Yan,

Zijian Zhou

et al.

Nano Letters, Journal Year: 2024, Volume and Issue: 24(18), P. 5444 - 5452

Published: April 19, 2024

We report, for the first time, a new synthetic strategy preparation of crystalline two-dimensional olefin-linked covalent organic frameworks (COFs) based on aldol condensation between benzodifurandione and aromatic aldehydes. Olefin-linked COFs can be facilely crystallized through either pyridine-promoted solvothermal process or benzoic anhydride-mediated flux synthesis. The resultant COF leaf with high in-plane π-conjugation exhibits efficient visible-light-driven photoreduction carbon dioxide (CO

Language: Английский

Citations

14