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Article
Chemistry, Multidisciplinary
Meng-Di Zhang et al.
Summary: In this study, a stable metal-organic framework (PcNi-Co-O) was reported as a bifunctional electrocatalyst for efficient CO2 overall splitting. PcNi-Co-O achieved a commercial-scale current density of 123 mA cm-2 and a Faradic efficiency (CO) of 98% at a low cell voltage of 4.4 V when used as both cathode and anode catalysts. Mechanism studies revealed the synergistic effects between two active sites and the energy-level matching of cathode and anode catalysts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Review
Chemistry, Multidisciplinary
Abhishek Dey
Summary: Reducing CO2 selectively to a specific C1 product is challenging due to similar thermodynamic reduction potentials for different CO2 reductions. Inspired by nickel CO dehydrogenase (Ni-CODH), the use of bimetallic iron porphyrins bridged by a urea moiety enables fast and selective reduction of CO2 to CO. The mechanism appears to mimic Ni-CODH, where one metal binds and reduces CO2 while the other stabilizes the reduced species and facilitates C-O bond cleavage.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Meng Lu et al.
Summary: In this work, dual photosensitizer-based three-dimensional metal-covalent organic frameworks (3D MCOFs) were successfully assembled by covalently linking pyridine ruthenium/ferrum (Ru(bpy)(3)(2+)/Fe(bpy)(3)(2+)) and porphyrin/metalloporphyrin complex (2HPor/ZnPor). These MCOFs demonstrated strong visible light-absorbing ability, efficient electron transfer, and suitable band gap, leading to highly efficient photocatalytic hydrogen (H-2) evolution. The Rubpy-ZnPor COF showed the highest H-2 yield (30,338 μmol g(-1) h(-1)) with an apparent quantum efficiency (AQE) of 9.68% at 420 nm, which is one of the best performances among all reported COF-based photocatalysts. Theoretical calculations revealed that both photosensitizer units in MCOFs can contribute to the optimal photocatalytic activity. This work establishes a general strategy and demonstrates the great potential of utilizing multiple photosensitive materials in the field of photocatalysis.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Keke Wang et al.
Summary: Researchers have developed a photocoupled electrocatalyst with high activity for CO2 reduction. The catalyst consists of aluminum-oxygen chains as the metal center and transition metal sites, and has achieved satisfactory CO2-to-CO conversion with a Faradaic efficiency as high as 90% and long-term stability over 35 hours under visible light. The improved performance is attributed to the stability provided by the aluminum-oxygen chains, the efficient charge transfer rate facilitated by the transition metal sites, and the accelerated charge transfer by visible light.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Multidisciplinary
Zhifeng Xin et al.
Summary: An oriented coordination strategy was reported to synthesize a series of site-specific functionalized electrocatalysts (HMTA@MOF-545-M) for efficient CO2 electroreduction. The HMTA@MOF-545-Co catalyst showed significantly enhanced CO2 adsorption-enthalpy and electrochemical active surface-area, resulting in almost twice higher CO2 electroreduction performance compared to the unmodified catalyst. The performance of HMTA@MOF-545-Co can be further improved under light-illumination, demonstrating high FECO, CO generation rate, and energy efficiency.
Article
Chemistry, Multidisciplinary
Qiu-Jin Wu et al.
Summary: We present the first example of a charged imidazolium functionalized porphyrin-based covalent organic framework for electrocatalytic CO2 reduction reaction. The free anions of imidazolium ions nearby the active sites can stabilize the key intermediate and inhibit hydrogen evolution reaction. Thus, the charged imidazolium functionalized covalent organic framework exhibits higher activity than the neutral version and follows a trend depending on the anion.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Engineering, Environmental
Li-Juan Gong et al.
Summary: Efficient charge transfer and photocatalytic CO2 reduction were achieved by integrating the photosensitizer [Ru(bpy)3]2+ and active cobalt porphyrin sites into a covalent organic framework (COF), named COF-RuBpy-Co. The catalyst COF-RuBpyCo exhibited excellent CO2 photoreduction activity with a rate of 547 mu mol g(-1)h(-1), which is a 1.4-fold enhancement compared to the physical mixture of Ru(bpy)(3)Cl-2 and COF-Bpy-Co. This study provides insights into the charge carrier transfer process and highlights the potential of COFs in artificial photosynthesis.
CHEMICAL ENGINEERING JOURNAL
(2023)
Review
Chemistry, Multidisciplinary
Changli Wang et al.
Summary: The electrocatalytic CO2 reduction reaction (ECO2RR) is an important approach to achieve lower carbon emissions in the future. The design of catalysts with satisfactory activity, selectivity, and stability for ECO2RR has attracted extensive attention. Functional porous frameworks, such as MOFs, COFs, composites, and pyrolysates, have been regarded as superior catalysts due to their unique properties. The structure-activity relationships of these frameworks have been comprehensively considered based on metallic element type, local coordination environment, and microstructure. The challenges and perspectives for further development of ECO2RR using functional porous frameworks are proposed in this review.
CHEMICAL SOCIETY REVIEWS
(2023)
Article
Chemistry, Physical
Shao-Shuai Zhao et al.
Summary: This study reports a series of 2D COFs based on thienothiophenes-porphyrin, which exhibit enhanced charge separation and migration for efficient photocatalytic conversion of CO2 under visible light irradiation. The π-π stacking interactions play an important role in COFs for CO2 conversion and provide insights into the mechanism of photocatalysis.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Multidisciplinary
Xiaozhi Li et al.
Summary: Efficient CO2 reduction reaction (CO2RR) in acidic electrolytes is achieved by manipulating mass transfer processes in well-designed hollow-structured Ag@C electrocatalysts, resulting in high faradaic efficiency and single-pass carbon efficiency. Computational modeling reveals that the unique structure of Ag@C regulates the diffusion process, creating a high-pH local reaction environment for enhanced activity. This work presents a promising route to engineer the microenvironment for high-performance CO2RR in acidic electrolytes.
Article
Chemistry, Multidisciplinary
Yuqiang Sheng et al.
Summary: A highly crystalline perylene imide supramolecular photocatalyst (PDI-NH) with breakthrough oxygen evolution rate and high quantum yield was synthesized via the imidazole solvent method. The highly crystalline structure is achieved through ordered self-assembly in molten imidazole solvent through pi-pi stacking and hydrogen bonding. The excellent performance is attributed to the robust built-in electric field, which accelerates charge separation and transfer. Furthermore, the catalyst is highly stable and can be reused.
ADVANCED MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Arghya Banerjee et al.
Summary: The study presents a visible-light-induced copper catalysis for the production of diverse heterocycles, with high tolerance to various functional groups. Preliminary mechanistic investigation suggests a cooperative action of two catalysts under visible-light irradiation to facilitate the reaction.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Wang Yao et al.
Summary: This research reports a strategy using excited-state palladium catalysis for the 1,2-radical migratory Mizoroki-Heck reaction, enabling C2-alkenylation of carbohydrates with 1-bromosugars and alkenes. The reaction shows tolerance to various functional groups and complex molecular architectures and expands the reactivity profile of excited-state Pd catalysis.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Review
Chemistry, Physical
Guobin Wen et al.
Summary: Electrochemical CO2 conversion is an attractive route for recycling CO2 with economic and environmental benefits, but further improvements are needed for catalytic materials and electrode structures; Electrocatalytic surface and near-surface engineering has the potential to enhance CO2 reduction reactions and specific strategies were proposed for improvement.
ADVANCED ENERGY MATERIALS
(2022)
Article
Engineering, Environmental
Shengtao Chen et al.
Summary: In this study, a novel Co-II-porphyrin/Ru-II-pincer complex coupled polymer was reported, which exhibited efficient visible light-responsive CO2RR activity. This work provides a new direction for exploring broadband-responsive covalent organic polymers with uniformly dispersed single-atom catalytic sites for CO2 photoreduction.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Nan Li et al.
Summary: This study presents a facile strategy to enhance the selectivity and current density of the electrochemical CO2 reduction reaction (CO2RR) by regulating the local electron density of bimetallic Co/Zn polyphthalocyanine frameworks. The optimal Co3Zn1PPc exhibits high CO partial current density and Faraday efficiency, indicating its potential for industrial applications.
Article
Chemistry, Multidisciplinary
Chang He et al.
Summary: This study reports the first stable CO2-masked N-heterocyclic carbenes (NHCs) grafted on a porous crystalline covalent organic framework (COF), and demonstrates their superior catalytic performances in hydrosilylation and N-formylation reactions. The NHC sites can be easily recycled and reused while maintaining excellent catalytic activity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Review
Chemistry, Inorganic & Nuclear
Shengsheng Huang et al.
Summary: Covalent organic frameworks (COFs) are a rapidly growing class of crystalline porous polymers that have a wide range of applications due to their unique features. By incorporating porphyrin (Por-) and phthalocyanine (Pc-) building units into COFs, they acquire unique structural characteristics and excellent optical and electrical properties. Recent progress has been made in the rational design and construction of Por- and Pc-based COFs for electrocatalytic water splitting, CO2 reduction, and oxygen reduction. This article provides a summary of the synthetic strategies of Por- and Pc-based COFs, an overview of their applications in electrocatalytic reactions, and discusses the current challenges and directions for further development.
COORDINATION CHEMISTRY REVIEWS
(2022)
Article
Chemistry, Multidisciplinary
Shaohong Wang et al.
Summary: Valence-inverted reactivity (VIR) is discovered through high-level computations of excited states of Ni(II) complexes that are generated by triplet energy transfer, and it plays a significant role in C-H bond activation and cross-coupling reactions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Jingyi Xu et al.
Summary: In this study, by incorporating carboxyl substituents into a novel oligomer, the charge separation and exciton transport of the photocatalyst have been improved, leading to efficient hydrogen and oxygen evolution. The high-performance oligomer photocatalyst provides a new approach for the production of solar fuel.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Review
Chemistry, Inorganic & Nuclear
Jintu Francis Kurisingal et al.
Summary: This article reviews recent progress in the design, synthesis, and catalytic mechanisms of COF-based functional materials for CO2 utilization reactions. It discusses various CO2 utilization reactions, such as photo/electrocatalytic CO2 reduction, cycloaddition, carboxylation, and hydrogenation, and evaluates the application of different types of COFs. The challenges and prospects of COF-based catalysts for CO2 utilization are highlighted.
COORDINATION CHEMISTRY REVIEWS
(2022)
Article
Chemistry, Multidisciplinary
Meng Lu et al.
Summary: This study designed a series of stable metallophthalocyanine COFs as novel single-site catalysts with outstanding activity and selectivity for electrocatalytic CO2 reduction. Coupled with light, these COFs showed improved efficiency and potential for applications in the field of electrocatalysis.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Ke Ye et al.
Summary: A strategy to in situ reconstruct a heterogeneous Ag2S/Ag interface structure is proposed for electrochemical CO2 reduction reaction, showing superior performance in terms of high current density and stable CO Faradaic efficiency. Density functional theory calculations reveal that the in situ reconstructive Ag2S/Ag interface active sites stabilize the *COOH intermediate during CO2RR process.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Environmental Sciences
Yi-Ming Wei et al.
Summary: A global layout for carbon capture, utilization, and storage (CCUS) is crucial for limiting global warming, with a proposed strategy matching carbon sources and sinks in 85 countries and regions. The findings show economic feasibility with identified carbon clusters and sinks, but global collaboration is needed for implementation.
NATURE CLIMATE CHANGE
(2021)
Article
Chemistry, Multidisciplinary
Yue Zhou et al.
Summary: Introducing an external light field can improve the efficiency of electrochemical CO2 reduction, with the synergistic effect of cationic Ti and additional light driving playing a key role in accelerating the process and promoting the conversion of CO2 to CO.
ADVANCED MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Jun Yang et al.
Summary: A full-spectrum responsive donor-acceptor supramolecular photocatalyst TPPS/C-60 was successfully constructed with high theoretical spectral efficiency. It achieved a highly efficient photocatalytic H-2 evolution rate and promoted charge separation efficiency. This work provides a novel approach for designing high-performance photocatalytic materials by enhancing the interfacial electric field.
ADVANCED MATERIALS
(2021)
Article
Chemistry, Physical
Gaurav Kumar et al.
Summary: This study explores the site-specific functionalization of sp3 C-H bonds adjacent to a nitrogen atom using a chemically robust COF material. The developed Ru-COF acts as a visible light photocatalyst for cross-dehydrogenative coupling reactions with excellent yield and functional group tolerance. The photocatalytic route is detailed through modulation of optical band-gap and validation of a single-electron-transfer pathway.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Physical
Hanjie Zhang et al.
Summary: This study demonstrates the critical influence of crystallinity and adjustments of the built-in electric field on the photocatalytic activity of PDI. The enhanced dipole and high degree of crystallinity of triazine-PDI enable a higher rate of photo-induced charge separation and transfer, resulting in improved phenol degradation and organic carbon removal rates compared to bulk g-C3N4 and supramolecular PDI.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Physical
Jun Han et al.
Summary: A series of porphyrin-based D-A type conjugated organic polymer nanotubes were synthesized via acid-catalyzed Schiff base reaction. Among them, CuTAPP-BT showed superior photocatalytic activity and recyclability for BPA degradation.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Multidisciplinary
Haozhou Yang et al.
Summary: A general synthetic method for zinc-metallophthalocyanine (MPc) molecular layer/polyoxometalate (POM) sandwich lamellar material was developed in this study, which improved the performance of CO2 reduction. The incorporation of POM prevented aggregation of MPc molecular layers and favored the exposure of active sites. The molecular layer sandwich catalyst showed superior CO2 reduction activity and achieved high CO Faradaic efficiency under dark and light conditions, with enhanced catalytic performance under external light field.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Wenpeng Ye et al.
Summary: The study demonstrates a chemical strategy for achieving high-performance blue phosphorescence by confining isolated chromophores in ionic crystals, forming high-density ionic bonds between the cations of ionic crystals and the carboxylic acid groups of the chromophores to create a segregated molecular arrangement with negligible inter-chromophore interactions.
Article
Chemistry, Physical
Geyla C. Dubed Bandomo et al.
Summary: The study presents a newly devised CO2 reduction catalyst by loading single-atom centers within a bipyridyl-based COF, showing improved catalytic performance. The findings can guide the rational development of isolated single-atom sites and the enhancement of catalytic performance in reticular materials.
Article
Chemistry, Multidisciplinary
Qiao Wu et al.
Summary: The TT-Por(Co)-COF, containing donor-acceptor heterojunctions, exhibits enhanced performance in electrocatalytic reduction of carbon dioxide to produce CO, thanks to its improved charge transfer capability and large amount of accessible active sites. This study demonstrates that integrating donor-acceptor heterojunctions in COFs can facilitate electron transfer and generate high current densities for CO2RR.
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Hong-Jing Zhu et al.
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Review
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Ying Hou et al.
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David M. Weekes et al.
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Christian S. Diercks et al.
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Christian S. Diercks et al.
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ADVANCED MATERIALS
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