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    Current Advances and Future Challenges of Single-atom Catalysis
    ZHUANG Jiahao, WANG Dingsheng
    Chem. J. Chinese Universities    2022, 43 (5): 20220043-.   DOI: 10.7503/cjcu20220043
    Abstract1454)   HTML71)    PDF(pc) (30735KB)(531)       Save

    Single-atom catalysts(SACs), which combines the advantages of homogeneous and heterogeneous catalysts, have attracted great research interest due to their maximum atomic utilization efficiency, superior catalytic performance and easy separation from reaction systems. However, due to the high surface energy and thus instability of single atoms, it remains a great challenge to rational design and fabricate stable SACs. In this review, we summarized and discussed the advances of stabilizing strategies, high-loading synthesis and batch preparation for SACs in recent years. We also envisioned the challenges on the future development of SACs. Finally, the research prospect of single-atom catalysis was forecasted.

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    Visible Light-driven Carboxylation with CO2
    ZHANG Zhen, DENG Yu, ZHANG Qinfang, YU Dagang
    Chem. J. Chinese Universities    2022, 43 (7): 20220255-.   DOI: 10.7503/cjcu20220255
    Abstract1384)   HTML76)    PDF(pc) (11197KB)(956)       Save

    Carbon dioxide(CO2) is not only a well-known greenhouse gas but also one important C1 resource. It is very important to realize organic transformations with CO2 to generate high value-added compounds. Given the importance of carboxylic acid and derivatives which are widely found in natural products, medicines, daily chemicals and industrial raw materials, the synthesis of carboxylic acids with CO2 has become an important research direction. On the other hand, high temperature and other harsh conditions are always required in this field due to the low reactivity of CO2. To solve such problems, visible light is used as an clean energy source to drive the effective transformations of CO2, which has been developed significantly in last few years. This review mainly introduced and summarized the visible light-driven carboxylation with CO2 in recent years, and classified them according to types of important chemical raw materials, such as alkenes, alkynes, aldehydes and ketones, imines organo(pseudo)halides and others. The characteristics and mechanisms of each reaction were discussed. In addition, this review also provided perspective to this emerging field.

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    Bio-chemical Synthesis of Melanin Precursor—— 5,6-Dihydroxyindole(DHI)
    JIN Ruiming, MU Xiaoqing, XU Yan
    Chem. J. Chinese Universities    2022, 43 (8): 20220134-.   DOI: 10.7503/cjcu20220134
    Abstract1115)   HTML26)    PDF(pc) (1746KB)(209)       Save

    In this study, the biological oxidation step for the synthesis of dopachrome(DC) from L-3,4-dihydroxyphenylalanine(L-Dopa) catalyzed by Saccharomyces cerevisiae BY4741/pYX212-TYR and the chemical step for the reductive synthesis of 5,6-dihydroxyindole(DHI) from DC were coupled, realizing the bio-chemical synthesis of DHI. By optimizing the reaction conditions and the oxygen supply strategy of the biological oxidation step, the conversion rate of L-Dopa increased to 94.75%; by optimizing the reaction conditions and chemical additives of the chemical reduction step, the yield of DHI increased to 90.03%. Ultra high performance liquid chromatography tandem quadrupole time of flight mass spectroscopy(UPLC-Q-TOF-MS) identification for the products showed that DHI-soluble oligomers existed in the reaction system.

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    Preparation and Performance of Paraffin/Expanded Graphite/Graphene Composite Phase Change Heat Storage Material
    YAN Jiasen, HAN Xianying, DANG Zhaohan, LI Jiangang, HE Xiangming
    Chem. J. Chinese Universities    2022, 43 (6): 20220054-.   DOI: 10.7503/cjcu20220054
    Abstract1032)   HTML27)    PDF(pc) (3231KB)(235)       Save

    The paraffin/expanded graphite/graphene aerogel composite phase change material was prepared by using paraffin(PA) as the phase change heat storage material, expanded graphite(EG) as the main thermal conductive material and support material, and graphene aerogel(GA) as the thermal conductivity enhancement material and auxiliary support material. The effects of the amount of GA added on the phase transition temperature, latent heat of phase transition, thermal conductivity and cycling stability of the composite material were investigated. The results show that the phase change material with composition of 80%PA-17%EG-3%GA has good thermal conductivity and excellent cycling stability. Compared with 80%PA-20%EG composite material, it exhibits almost the same phase transition temperature, latent heat of phase transition and cycling stability, but increased thermal conductivity from 4.089 W/(m·K) to 5.336 W/(m·K), showing good application prospects.

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    Electrocatalytic CO2 Reduction over Single-atom Catalysts
    JIN Xiangyuan, ZHANG Libing, SUN Xiaofu, HAN Buxing
    Chem. J. Chinese Universities    2022, 43 (5): 20220035-.   DOI: 10.7503/cjcu20220035
    Abstract938)   HTML62)    PDF(pc) (13736KB)(855)       Save

    Electrochemical CO2 reduction reaction(e-CO2RR) is a promising and facile method to achieve carbon-neutral economy and sustainable development due its simple device and capability to consume renewable energy to produce high value-added chemicals. However, e-CO2RR suffers from low selectivity and low current density because of its sluggish kinetics and the weak activity of the catalysts. Hence, single-atom catalysts are one of the most ideal materials for e-CO2RR by virtue of its maximum atom utilization and well-defined catalytic active sites. Single atoms derived from transition metal and main group metal are comprehensively reviewed. Heteroatom coordination, dual-atom site, metal-support interactions, spatial confinement and molecular bridging to tailor the microenvironment of single atom to realize a better catalytic performance are also included. Single-atom catalysts extremely accelerate electrocatalytic CO2 reduction kinetics, which is ascribed to its unique electronic structure and enormous intrinsic highly active sites, indicating its state-of-the-art merits and broad application prospects. Reductive products that involve multi-electrons are desired for single-atom catalysts. Finally, research trends and hotspots in this field are also discussed.

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    Research Progress of Single-atom Catalysts in Photocatalytic Reduction of Carbon Dioxide
    TAO Yu, OU Honghui, LEI Yongpeng, XIONG Yu
    Chem. J. Chinese Universities    2022, 43 (5): 20220143-.   DOI: 10.7503/cjcu20220143
    Abstract930)   HTML43)    PDF(pc) (10632KB)(478)       Save

    The conversion of carbon dioxide into value-added carbon-containing chemicals or fuels through photo-catalytic technology is one of the sustainable ways to solve the energy crisis and greenhouse effect. However, it is a great challenge to pursue catalysts with high efficiency, low price, and high stability for improving the efficiency of photocatalytic reduction reaction of CO2(CO2RR). Single atom catalysts(SACs) have been widely studied in the field of catalysis because of their high atomic utilization and adjustable electronic environment. In photocatalysis of CO2RR, the addition of single metal atoms can not only adjust the energy band structure and the light adsorption ability of catalysts, but also effectively improve the efficiency of photogenerated charge transfer, and provide an ideal platform for the study of photocatalytic reaction mechanism. In recent years, the research of SACs in CO2RR has developed rapidly. In this paper, the progress of SACs of photocatalytic CO2RR is summarized, and the typical research results of SACs with different supports are introduced, and the future research trend is prospected.

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    Recent Progress in Heterogeneous Catalysts for the Hydrogenation of Carbon Dioxide to Methanol
    ZHOU Zixuan, YANG Haiyan, SUN Yuhan, GAO Peng
    Chem. J. Chinese Universities    2022, 43 (7): 20220235-.   DOI: 10.7503/cjcu20220235
    Abstract900)   HTML68)    PDF(pc) (12477KB)(842)       Save

    The utilization of fossil fuels has enabled an unprecedented era of prosperity and advancement of well- being for human society. However, the associated increase in anthropogenic carbon dioxide(CO2) emissions can negatively affect global temperatures and ocean acidity. Moreover, as a limited resource, the depletion of fossil fuels will ultimately force one to seek alternative carbon sources to maintain a sustainable development. Using green hydrogen obtained from the water electrolysis process carried out using electricity generated from renewable sources, the hydrogenation of captured CO2 to methanol not only efficiently utilizes the excess effluent CO2 from industrial gaseous waste, but also produces a clean and renewable chemical feedstock of methanol, the core of which is to develop highly efficient and stable catalysts for methanol formation. In this review, we discuss the reaction mechanism and structure-activity relationship of common heterogeneous catalysts for CO2 hydrogenation to methanol which has attracted great attention in the past decades. We also review the latest development in the design and synthesis of heterogeneous catalysts(Cu-based catalyst, noble metal catalyst and bimetallic catalysts, oxide catalyst and other novel catalysts) for methanol synthesis through the direct hydrogenation of CO2. Moreover, the opportunities and challenges in this field are also prospected.

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    Modified Quasichemical Model for Manifold Short-range Orders in Binary Solutions: Unity of Opposites for the Ordered Pairs
    WANG Kun, ZOU Xingli, CAO Zhanmin, LI Chonghe, LU Xionggang
    Chem. J. Chinese Universities    2022, 43 (11): 20220391-.   DOI: 10.7503/cjcu20220391
    Abstract888)   HTML11)    PDF(pc) (1164KB)(150)       Save

    Within the framework of the quasichemical model, assuming all ordered pairs of atoms to be distingui-shable, a modified quasichemical model for twofold short-range orders(SROs) was firstly constructed, and then several theoretical limits that the model can reach were discussed. These discussions were summarized and enhanced to establish the theory of unity of opposites for ordered pairs. Based on this theory, the modified quasichemical model for twofold SROs were further generalized, which leads to the successful development of the modified quasichemical model for manifold SROs. The model can efficiently describe the thermodynamic behavior of binary melts containing manifold short-range ordering configurations. The Bi-K melt with at least two observed SROs were selected to test the rationality and reliability of the model. The results show that, apart from the coordination numbers, only four model parameters are needed to reasonably reproduce all the thermochemical data of the binary melt.

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    Ordered Mesoporous Materials: History, Progress and Perspective
    GUO Cheng, ZHANG Wei, TANG Yun
    Chem. J. Chinese Universities    2022, 43 (8): 20220167-.   DOI: 10.7503/cjcu20220167
    Abstract849)   HTML43)    PDF(pc) (21747KB)(658)       Save

    Ordered mesoporous materials with pore diameters ranged from 2 nm to 50 nm possess ordered mesostructures, high surface areas, large pore volumes and tunable compositions, which have received great research interests in many fields. In the past decades, the precise synthesis, rational design, and controllable functionalization of ordered mesoporous materials have made great progresses, thereby laying a solid foundation for the practical applications, including energy storage and conversion, catalysis, biomedicine, and sensing. This review first summarizes the development history of ordered mesoporous materials comprehensively, and the milestones in this field are reviewed in detail. After that, based on the structure-property relationship, the latest progresses of ordered mesoporous materials in emerging fields, such as energy, catalysis and biomedicine are overviewed. In the last, the research challenges in this field are presented and the future perspectives are outlined.

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    Research Progress of Zeolite-encaged Single-atom Metal Catalysts
    LI Jiafu, ZHANG Kai, WANG Ning, SUN Qiming
    Chem. J. Chinese Universities    2022, 43 (5): 20220032-.   DOI: 10.7503/cjcu20220032
    Abstract800)   HTML29)    PDF(pc) (13025KB)(471)       Save

    Zeolites are considered as ideal supports for encapsulating ultrasmall metal species due to their uniform microporous channels, large specific surface areas, and excellent thermal stability. In recent years, thanks to the superhigh metal dispersion, nearly 100% metal utilization efficiency and unique electronic structure, zeolite-encaged single-atom metal catalysts have been widely used in many important catalytic reactions and gas adsorption/separation processes. In this review, we present a comprehensive summary of the state-of-the-art synthetic strategies of zeolite-encaged different kinds of single-atom metal catalysts and their applications in heterogeneous catalysis and gas separation. In the last part of this review, some future perspectives on the challenge and opportunity for this subject are pointed out. We hope that this review will provide reference for researchers to carry out more innovative research works in the future.

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    Progress of CO2 Electroreduction to Oxalic Acid
    SONG Dewen, WANG Mingwang, WANG Yani, JIAO Zhenmei, NING Hui, WU Mingbo
    Chem. J. Chinese Universities    2022, 43 (7): 20220248-.   DOI: 10.7503/cjcu20220248
    Abstract787)   HTML51)    PDF(pc) (4807KB)(674)       Save

    In recent years, climate issues such as global warming caused by excessive carbon dioxide emissions have attracted wide attention around the world. And carbon emission reduction has become a common challenge to the sustainable development of human society. The conversion of carbon dioxide into high value-added chemicals by electrochemical methods is one of the ideal ways to achieve emission reduction and high value-added utilization of carbon dioxide. However, there are still many problems such as high energy consumption, low carbon dioxide conversion, poor product selectivity and difficult separation. In this paper, we take the electroreduction of carbon dioxide to oxalic acid as an example, comprehensively introduce the research progress from the aspects of reaction mechanism, catalysts, electrolyte, electrode and reactor. The key problems in the production of oxalic acid by carbon dioxide electroreduction are discussed and some valuable suggestions are put forward for the future research of carbon dioxide electroreduction to oxalic acid.

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    Single-atom and Cluster Photocatalysis: Competition and Cooperation
    LIN Zhi, PENG Zhiming, HE Weiqing, SHEN Shaohua
    Chem. J. Chinese Universities    2022, 43 (9): 20220312-.   DOI: 10.7503/cjcu20220312
    Abstract737)   HTML24)    PDF(pc) (7157KB)(327)       Save

    Photocatalytic technology has been considered as a promising and sustainable technology to convert solar energy to storable chemical energy. With active sites(single metal atoms and clusters) atomically dispersed on the semiconductor, the mass and charge transfer in photocatalysis can be significantly promoted, and the photocatalytic performance can be remarkably improved. However, it is still controversial whether clusters or single-atoms are the real active sites in catalysts. In this review, the recent advances in single-atom photocatalysis are briefly introduced, with the competition and synergy of single-atoms and clusters analyzed and discussed. Then, the state-of-the-art technologies in the identification and characterization of single-atoms and clusters as photocatalytic active sites are presented. Finally, the future development of single-atoms/clusters synergistic photocatalysis in solar-chemical energy conversions such as water splitting and CO2 reduction is prospected.

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    Progress on the Stereocontrolled Synthesis of Phosphorothioate Oligonucleotides
    CAO Shujie, LI Hongjun, GUAN Wenli, REN Mengtian, ZHOU Chuanzheng
    Chem. J. Chinese Universities    2023, 44 (3): 20220304-.   DOI: 10.7503/cjcu20220304
    Abstract721)   HTML12)    PDF(pc) (3881KB)(335)       Save

    Phosphorothioate(PS) oligonucleotides have found a wide range of applications in biochemical mechanism studies, biomedicine, materials and related fields. The stereo configuration of PS has a remarkable effect on the biochemical properties of PS nucleic acids, which has aroused wide interest in developing methods for efficient and stereoselective synthesis of PS oligonucleotides in the past 30 years. This review summarized the methods for stereocontrolled synthesis of PS oligonucleotides, with a focus on the research progress in the past decade. The advantages and disadvantages of different methods were comparatively analyzed. Finally, the prospect of stereocontrolled synthesis of PS oligonucleotides was briefly discussed.

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    A Dataset Representativeness Metric and A Slicing Sampling Strategy for the Kennard-Stone Algorithm
    WU Qingying, ZHU Zhenyu, WU Jianming, XU Xin
    Chem. J. Chinese Universities    2022, 43 (10): 20220397-.   DOI: 10.7503/cjcu20220397
    Abstract704)   HTML6)    PDF(pc) (1847KB)(115)       Save

    In machine learning with big data, it is essential to prepare a representative dataset for training a model. The Kennard-Stone(KS) algorithm and its derivatives are a large class of excellent dataset splitting methods. But it rely heavily on empirical selection or modeling results to determine the sampling ratio and sampling number. In addition, its computational complexity is OK3? according to the original literature, making it difficult to apply to massive data. In this paper, we design a metric based on dataset completeness to quantify the representativeness degree of an extracted subset to the whole dataset. An amendment using dynamic programming algorithm is put to reduce the algorithm complexity to O'K2. And a slicing sampling strategy is proposed to divide the whole dataset into several subset and implement KS sampling respectively, which can further improve the algorithm efficiency to O''K. The partial least squares regression test results show that the method can improve the sampling efficiency while still ensuring the representativeness of the finally extracted dataset.

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    Efficient Electrocatalytic CO2 Reduction over Pyrrole Nitrogen-coordinated Single-atom Copper Catalysts
    ZHAO Runyao, JI Guipeng, LIU Zhimin
    Chem. J. Chinese Universities    2022, 43 (7): 20220272-.   DOI: 10.7503/cjcu20220272
    Abstract684)   HTML36)    PDF(pc) (4149KB)(256)       Save

    A series of carbon nanotube supported copper single-atom catalysts(SACu/CNT-x) was synthesized by a temperature-controlled impregnation-pyrolysis method. Extended X-ray absorption fine structure(EXAFS) analysis indicates that the single-atom copper sites were coordinated with pyridinic-N and pyrrolic-N, respectively, in the catalysts. The catalysts were applied in electrocatalytic carbon dioxide reduction. It was indicated that the catalyst with pyrrole N-coordinated copper single-atom sites showed high activity for CO2 electroreduction, affording a high CO Faradaic efficiency of 96.3% at -0.70 V(vs.RHE). Electrochemical experiments show that the pyrrole N-coordinated copper single-atom center has a good inhibitory effect on the hydrogen evolution reaction.

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    Recent Advances in Single-atom Materials for Enzyme-like Catalysis and Biomedical Applications
    SHA Meng, XU Weiqing, WU Zhichao, GU Wenling, ZHU Chengzhou
    Chem. J. Chinese Universities    2022, 43 (5): 20220077-.   DOI: 10.7503/cjcu20220077
    Abstract668)   HTML27)    PDF(pc) (14879KB)(493)       Save

    Nanozymes featuring with economic cost, high stability, tunable properties, have captured broad interest to break through the limitations of enzymes in practice. The emergency of single-atom materials pushes forward the nanozymes research into the atomic level. Single-atom materials with high atomic utilization efficiency, unique coordination environments and strong metal-support interactions offer great opportunities to reveal their structure-activity relationship and regulate their enzyme-like activities. In this review, recent advances of single-atom materials for enzyme mimicking and biomedical applications were depicted. First, the regulation strategies and catalytic mechanisms of enzyme-like activities were discussed in detail. Then, the applications of single-atom nanomaterials for enzyme mimicking were elucidated in terms of cancer treatment, antioxidant therapy, antibacterial and biosensing. Finally, the limitations, challenges and development prospects of single-atom nanomaterials for enzyme-like catalysis were proposed.

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    Application of DNA Silver Nanoclusters in the Fluorescence Biosensors based on Functional Nucleic Acids
    WANG Junyang, LIU Zheng, ZHANG Qian, SUN Chunyan, LI Hongxia
    Chem. J. Chinese Universities    2022, 43 (6): 20220010-.   DOI: 10.7503/cjcu20220010
    Abstract646)   HTML412)    PDF(pc) (10068KB)(540)       Save

    DNA silver nanoclusters(DNA-AgNCs) are a kind of fluorescent nanoprobes obtained by reducing Ag+ with NaBH4 using DNA as template, because the N atoms on the base heterocyclic are combined with Ag+. Due to the advantages of simple synthesis method, good biocompatibility and adjustable fluorescence emission wavelength, DNA-AgNCs have been widely used in the fields of analysis and detection. In this paper, the application of DNA-AgNCs as label-free fluorescent probes in functional nucleic acids biosensing detection is classified and summarized. In addition, conclusive views on the deficiencies and application potential are put forward, which provide references for future research and application.

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    Progress in the Structure Design and Surface Manipulation of Lithium-rich Cathode Materials
    ZHAO Xiaolang, YANG Mei, WANG Jiangyan, WANG Dan
    Chem. J. Chinese Universities    2023, 44 (1): 20220263-.   DOI: 10.7503/cjcu20220263
    Abstract626)   HTML10)    PDF(pc) (20007KB)(357)       Save

    Lithium-rich cathode materials are regarded as promising cathode candidates for next-generation lithium-ion battery, due to their high theoretical energy density. However, the rapid capacity and voltage decay during cycling hinders their practical commercial application. In this review, the research progress of improving the lithium storage performance of lithium-rich cathode materials through structure design and surface manipulation was summarized in detail. Firstly, the working mechanism of charge and discharge of lithium-rich cathode materials as well as the reasons for their specific capacity and voltage decay were introduced. Subsequently, we discussed the recent progress in improving the performance of lithium-rich cathode materials through novel structural design and surface manipulation strategies. By constructing novel structure such as yolk-shell and hollow multishelled structure, and by controlling the particle size, exposing beneficial surface, surface spinelization, surface coating, surface doping, etc., the surficial oxygen loss and crystal form transformation of the lithium-rich cathode materials could be effectively inhibited, and the geometric structure could be stabilized. As a result, the decay of voltage and specific capacity could be suppressed, and the cycle life and Coulomb efficiency of the battery could be improved. Finally, the remained challenges of improving the electrochemical performance of lithium-rich cathode materials are discussed and the future development directions are prospected.

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    Applications of Single-atom Catalysts in CO2 Conversion
    QIN Yongji, LUO Jun
    Chem. J. Chinese Universities    2022, 43 (9): 20220300-.   DOI: 10.7503/cjcu20220300
    Abstract626)   HTML37)    PDF(pc) (18664KB)(318)       Save

    Single-atom catalyst(SAC), emerging as a kind of promising catalyst materials with isolated active sites anchored on diverse matrixes, has shown excellent performances in thermocatalysis, photocatalysis and electrocatalysis due to their maximized efficiency of atoms and unique, adjustable electronic structure. Among all the reactions catalyzed by SAC, thermo/photo/electrocatalytic CO2 conversion reaction(CCR) converts CO2, the greenhouse gas, into fuels or value-added chemicals, which provides an effective strategy for solving the serious issues of global warming and energy shortage. In this perspective, based on the catalytic conversion of CO2 by SAC, the research progresses in the field of CO2 conversion reaction by SAC in recent years are summarized, the advantages and disadvantages of the synthetic methods, regulation and various CCRs are discussed, and the future development of SAC is prospected.

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    Visible-light-driven Selective Reduction of Carbon Dioxide Catalyzed by Earth-abundant Metalloporphyrin Complexes
    QIU Liqi, YAO Xiangyang, HE Liangnian
    Chem. J. Chinese Universities    2022, 43 (7): 20220064-.   DOI: 10.7503/cjcu20220064
    Abstract619)   HTML28)    PDF(pc) (8391KB)(483)       Save

    With the increasing energy shortage and environmental problems, the search for clean and renewable energy sources to replace fossil fuels is one of the most urgent tasks facing scientists in this century. In order to achieve our "carbon neutrality" strategic goal, the conversion of carbon dioxide(CO2) into clean fuels and chemicals using solar energy is one of the ways to achieve the sustainable development of our society. The catalyst is the core component of CO2 photoreduction technology, which can adsorb gaseous CO2 molecules and reduce them to small energy molecules such as carbon monoxide(CO), formic acid(HCOOH), methanol(CH3OH) and methane(CH4) under visible light irradiation. Currently, promising progress has been made in the development of novel CO2 reduction photocatalytic systems. This review summarizes the recent progress of homogeneous and heterogeneous earth-abundant metalloporphyrin-based catalysts for photocatalytic CO2 reduction, and introduces the reaction mechanism of CO2 photoreduction to CO or CH4 by homogeneous metalporphyrin catalysts, respectively, and also discusses the important applications of metalloporphyrin-based porous organic polymers with porphyrin organometallic frameworks for photocatalytic CO2 reduction. Finally, the prospect of visible-light-driven metalloporphyrin complex-catalyzed CO2 reduction is presented.

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