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Metal-organic frameworks with dinuclear metal centers for synergistically boosting CO2 photoreduction

Science China Chemistry 2025年第1期 201-208页

作者： Hui-Feng Wang Wen-Jie Shi Yu-Xin Yang Bao-Xia Dong Tong-Bu Lu di-chang zhong School of Chemistry and Chemical Engineering Yangzhou University Institute for New Energy Materials and Low Carbon Technologies School of Materials Science and Engineering Tianjin University of Technology

dinuclear metal synergistic catalysis （DMSC） has been proved powerful in boosting CO2reduction,while this has not been achieved in heterogeneous catalysts with long-range order *** this study,we,by introduction of metal catalytic centers into an indium-based metal-organic framework （MOF）,obtained a series of isostructural In-MOFs,including three MOFs with mononuclear metal catalytic center （M-In）,three MOFs with dinuclear homometallic catalytic centers （MM-In）,and three MOFs with dinuclear heterometallic catalytic centers (MM’-In,M/M’=Co（II）,Ni（II）,Zn（II）).It was found that all these MOFs can serve as catalysts for photochemical CO2reduction to *** with M-In,the catalytic activities of MM-In were obviously enhanced,and that of MM’-In was further significantly *** example,the CO yield of Co Zn-In reaches a record value of 12,700μmol g-1h-1,which is 4.0,8.1,9.4,and 18.6-fold higher than that of Co Co-In,Zn Zn-In,Co-In,and Zn-In,***,the catalytic activities of Co Ni-In and Ni Zn-In also show different fold increase than those of corresponding dinuclear homometallic and mononuclear metallic *** results of control experiments and theoretical calculation reveal that the higher catalytic activities of MM-In over M-In can be ascribed to the DMSC effect,and the higher catalytic activity of MM’-In over MM-In can be ascribed to the strengthened DMSC *** work reveals the relationship between DMSC effect and bimetal centers in CO2reduction,which provides new insights into the DMSC and paves a new way to design highly active catalysts for photochemical CO2reduction.

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Integration of metal-organic layers with quantum dots for artificial photosynthesis

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Science China Chemistry 2024年第11期67卷 3712-3718页

作者： Hong Yuan Min Zhang Ji-Hua Deng Tong-Bu Lu di-chang zhong Institute for New Energy Materials and Low Carbon Technologies School of Materials Science and EngineeringSchool of Chemistry and Chemical EngineeringTianjin University of TechnologyTianjin 300384China

Metal-organic layers(MOLs), a type of new-emerging two-dimensional ultrathin metal-organic framework materials with large surface areas and highly exposed active sites, have shown promising applications in photocatalytic CO_(2) reduction. However, due to a lack of photosensitivity and photooxidation capability, photosensitizers and sacrificial reductants are usually necessary for MOLs-based photocatalytic CO_(2) reduction systems. In this article, by integration of MOLs and quantum dots(QDs), we constructed MOLs-based catalysts with multi-functions of photosensitivity, photoreduction and photooxidation, which thus can serve as photocatalysts for CO_(2) reduction with H_(2)O as an electron donor. Specifically, by an electrostatic self-assembly approach,nickel(Ⅱ)-based MOLs(Ni-MOLs) and CsPbBr_(3)QDs have been assembled, constructing valid Ⅱ-Scheme Ni-MOLs/CsPbBr_(3) heterojunctions with close Ni-MOLs/CsPbBr_(3)heterointerface. Such a close heterointerface shortens the charge transfer distance,thus effectively boosting the charge separation and transfer. As a result, upon illumination by visible light(λ ≥ 400 nm,100 m W cm^(-2)), the optimized photocatalyst shows high efficiency and stability in photochemical CO_(2) reduction in the absence of any photosensitizers and sacrificial reductants. The CO yield reaches as high as 124 μmol g^(-1)in 4 h, over 6 times higher than that achieved by CsPbBr_(3). Additionally, the selectivity reaches 100%. This work provides a new way to construct MOL-based catalysts for artificial photosynthesis.

关键词： metal-organic layers artificial photosynthesis CO_(2)reduction H_(2)O oxidation

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Facile synthesis of C_(3)N_(4)-supported metal catalysts for efficient CO_(2) photoreduction

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Nano Research 2022年第1期15卷 551-556页

作者： Yun-Nan Gong Bi-Zhu Shao Jian-Hua Mei Wei Yang di-chang zhong Tong-Bu Lu Institute for New Energy Materials and Low Carbon Technologies School of Materials Science and EngineeringSchool of Chemistry and Chemical EngineeringTianjin University of TechnologyTianjin 300384China Key Laboratory of Jiangxi University for Functional Material Chemistry College of Chemistry&Chemical EngineeringGannan Normal UniversityGanzhou 341000China

Facile synthesis of photocatalysts with highly dispersed metal centers is a high-priority target yet still a significant *** this work,a series of Co-C_(3)N_(4) photocatalysts with different Co contents atomically dispersed on g-CaN4 have been prepared via one-step thermal treatment of cobalt-based metal-organic frameworks(MOFs)and urea in the *** to the highly dispersed and rich exposed Co sites,as well as good charge separation efficiency and abundant mesopores,the optimal 25-Co-C_(3)N_(4),in the absence of noble metal catalysts/sensitizers,exhibits excellent performance for photocatalytic C0_(2) reduction to CO under *** irradiation,with a high CO evolution rate of 394.4μmol·g^(-1)·h^(-1),over 80 times higher than that of pure g-C_(3)N_(4)(4.9μmol·g^(-1)·h^(-1)).In:addition,by this facile synthesis strategy,the atomically dispersed Fe and Mn anchoring on g-C_(3)N_(4)(Fe-C_(3)N_(4) and Mn-C_(3)N_(4))have been also obtained,indicating the reliability and universality of this strategy in synthesizing photocatalysts with highly dispersed metal *** work paves a new way to develop cost-effective photocatalysts for photocatalytic C0_(2) reduction.

关键词： metal-organic frameworks highly dispersed metal g-C_(3)N_(4) photocatalysts C02 reduction

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Cobalt-based heterogeneous catalysts for photocatalytic carbon dioxide reduction

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Tungsten 2024年第2期6卷 410-421页

作者： Hong Yuan Jian-Hua Mei Yun-Nan Gong di-chang zhong Tong-Bu Lu MOE International Joint Laboratory of Materials Microstructure Institute for New Energy Materials and Low Carbon TechnologiesSchool of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China

Solar light-driven CO_(2)reduction to high value-added chemicals has considered as an outstanding way to solve energy crisis and climate ***,various photocatalysts have been developed to achieve this *** them,cobaltbased heterogeneous catalysts have attracted great interest because of their promising performance,product selectivity and ***,we systematically summarize the research progress of various cobalt-based heterogeneous catalysts for the photoreduction of CO_(2),such as single-atom cobalt,and cobalt-based oxides,nitrides,sulfi des,phosphides,metal-organic frameworks and covalent-organic ***,the advantages and structure-activity relationship of these catalysts in photocatalytic CO_(2)reduction reaction are ***,the challenges and prospects for constructing cobaltbased heterogeneous catalysts with high effi ciency are highlighted.

关键词： Cobalt Heterogeneous catalysts CO_(2)reduction Photocatalysis

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Boosting photocatalytic CO2-to-CO conversion using a biomimetic dinuclear Co（II） complex through an HCO3--mediated pathway

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Science China Chemistry 2024年

作者： Yuchen Wang Wenjie Shi Weixue Tao Jihong Zhang di-chang zhong Tongbu Lu Institute for New Energy Materials and Low Carbon Technologies School of Materials Science and EngineeringTianjin University of Technology

dinuclear metal synergistic catalysis（DMSC） has been evidenced to be effective in enhancing the catalytic activity for CO2reduction. However, the reaction kinetics of CO2reduction is still limited by the local CO2concentration around the dinuclear catalytic centers. Inspired by the structure of carbonic anhydrase, we have designed and synthesized a dinuclear cobalt（II）complex with an -OH group. This complex not only exhibits DMSC for CO2reduction but also possesses excellent capture capacity for CO2molecules. Consequently, the complex demonstrates high efficiency for the photocatalytic reduction of CO2to CO, with turnover number reaching as high as 43,400 and a selectivity of 97%. Even in 10% CO2, the complex still shows state-of-the-art catalytic activity. The results of experiments and theoretical calculations reveal that besides the DMSC contributing to the enhanced catalytic activity, the -OH group in the dinuclear cobalt（II） complex facilitates the capture of CO2by the formation of HCO3-intermediates, thereby enhancing the affinity towards CO2and boosting the catalytic activity for CO2-to-CO conversion.

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A Two-Fold Interpenetrating Porous Metal–Organic Framework with Large Solvent-Accessible Volume: Gas Sorption and Luminescent Properties

A Two-Fold Interpenetrating Porous Metal–Organic Framework ...

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中国化学会第九届全国无机化学学术会议

作者： Yun-Nan Gong di-chang zhong Key Laboratory of Jiangxi University for Functional Material Chemistry College of Chemistry ＆ Chemical Engineering Gannan Normal University

Porous metal-organic frameworks（MOFs） have been given great attention not only due to their intriguing structures and diverse topologies, but also due to their potential applications in gas storage and separation,ion-exchange, catalysis, and molecular sensing.[1-3] Herein, we have successfully synthesized a new two-fold interpenetrating luminescent porous metal-organic framework with large solvent-accessible volume of 51% per unit cell volume. The compound exhibits gas sorption behaviors for N2, H2 and CO2 gases. Furthermore, it also shows guest-responsive luminescent changes toward different solvent molecules.

关键词： Metal-organic frameworks two-fold interpenetrating gas sorption molecular sensing

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Molecular Cloning of a Novel Mouse Testis-specific Spermatogenic Cell Apoptosis Inhibitor Gene mTSARG7 as a Candidate Oncogene

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Acta Biochimica et Biophysica Sinica 2005年第6期37卷 396-405页

作者： Xiao-Jun TAN Xiao-Wei XING Lu-Yun LI Zhao-di WU chang-Gao zhong Dong-Song NIE Jun-Jiang FU Yang XIANG Yun DENG Guang-Xiu LU Institute of Human Reproductive and Stem cell Engineering, Central South University, changsha 410078,China Institute of Human Reproductive and Stem cell Engineering Central South University Changsha 410078 China

A novel mouse gene,mTSARG7(GenBank accession ***489184),with a full cDNA lengthof 2279 bp and containing 12 exons and 11 introns,was cloned from a mouse expressed sequence tag(GenBank accession ***644543)that was significantly up-regulated in *** gene waslocated in mouse chromosome 8A1.3 and encoded a protein containing 403 amino acid residues that was anew member of the acyltransferase family because the sequence contained the highly conserved phosphateacyltransferase(PlsC)domain existing in all acyltransferase-like *** mTSARG7 protein and AU041707protein shared 83.9% identity in 402 amino acid *** of the mTSARG7 gene was restrictedto the mouse *** results of the in situ hybridization analysis revealed that the mTSARG7 mRNA wasexpressed in mouse spermatogonia and *** localization studies showed that the EGFP-tagged mTSARG7 protein was localized in the cytoplasm of GC-1 spg *** mTSARG7 mRNA expres-sion was initiated in the mouse testis in the second week after birth,and the expression level increasedsteadily with spermatogenesis and sexual maturation of the *** results of the heat stress experimentshowed that the mTSARG7 mRNA expression gradually decreased as the heating duration ***3.1 Hygro(-)/mTSARG7 plasmid was constructed and introduced into GC-1 spg cells by *** mTSARG7 can accelerate GC-1 spg cells,causing them to traverse the S-phase and enterthe G2-phase,compared with the control group where this did not occur as there was no transfection *** conclusion,our results suggest that this gene may play an important role in spermatogenesisand the development of cryptorchid testes,and is a testis-specific apoptosis candidate oncogene.

关键词： mTSARG7 testis spermatogenesis oncogene

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Photocatalytic reduction of CO2 to CO with molecular Co(Ⅱ) complexes

Photocatalytic reduction of CO2 to CO with molecular Co(Ⅱ) ...

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中国化学会第八届全国配位化学会议

作者： Ting Ouyang Ke-Jun Wang di-chang zhong Tong-Bu Lu School of Chemistry & Chemical Engineering Gannan Normal University Institute for New Energy Materials and Low Carbon Technologies Tianjin University of Technology

The use of sunlight and catalysts to convert carbon dioxide(CO) into chemical fuels and feedstocks have attracted tremendous scientific interests for two main reasons:the shortage of energy and the problem of global warming.[1]To achieve both purposes,the development of artificial photosynthetic systems from which solar fuels can be produced from CO and HO is essential. The past investigations have shown that the reduction products of CO usually include CO,formic acid,methane,methanol,and oxalate,of which getting a single reduction production of CO has attracted particular ***,we report a Co(Ⅱ)-based homogeneous catalyst,[Co(NTB)CHN](CIO)(Co,NTB=tris(benzimidazolyl-2-methyl)amine,Figure la),which shows high efficiency,selectivity and stability for the catalytic reduction of CO to CO in a water-containing system driven by visible-light,with turnover number(TON) and turnover frequency(TOF) values of 1179 and 0.032 s,respectively,and selectivity to CO of 97%.And we also report a dinuclear cobalt cryptate,[Co(OH)L](ClO)(CoCo),as a catalyst for the photocatalytic reduction of CO to CO(L=N[(CH)NHCH(mCH)CH-NH-(CH)]N,see Figure 1b),with turnover number(TON) and turnover frequency(TOF)values of 1179 and 0.032 s,and selectivity to CO of 97%.respectively,and selectivity to CO of97%.

关键词： homogeneous photocatalyst CO2 reduction Co(Ⅱ)-Based complex cryptand

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Anion-dependent formation of four coordination polymers based on N,N'-di(3-pyridine) oxamide(DPOM)

Anion-dependent formation of four coordination polymers base...

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中国化学会第八届全国配位化学会议

作者： Ya-Qiong Wen Ji-Hua Deng Ping Lian di-chang zhong School of Chemistry & Chemical Engineering Gannan Normal University

With intriguing structures and potential applications in the fields of photoluminescence,catalysis,molecular magnet,and so on,coordination polymers(CPs) have continuously attracted widespread attention over the past several decades.[1-2]For constructions of CPs with neutral organic ligands,the anions associated with the metal ions will inevitably be incorporated into the framework to balance the charges of the whole CP *** may act as terminal ligands to occupy some of the coordination sites,or may serve as versatile linkers to connect metal ions into more complicated structural units such as metal clusters,thereby producing new coordination polymers[3].In this context,it is necessary to investigate the correlation between the anion and structure,which is beneficial to interpret the law of self-assemble in coordination polymers and create new desired CP ***,we designed a new amide ligand,N,N’-di(3-pyridine)oxamide ligand(DPOM) and reported the crystal structures and luminescent properties of four coordination polymers with DPOM,including two one-dimensional(1 D) chain/ladder polymers,[Ni(DPOM)(H O)]SO·2 H O(1) and[Cd(DPOM)(NO)](2),as well as two 3 D coordination polymers,[Zn(DPOM)(H O)(SO)](3) and[Cd(DPOM)(H O)(SO)](4).

关键词： coordination polymers N,N’-di(3-pyridine) oxamide (DPOM) anion-dependent photoluminescent property

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Syntheses,crystal structures,and crystal to crystal transformation of Three supramolecular compounds of 1,4-benzeneditetrazole

Syntheses,crystal structures,and crystal to crystal transfor...

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中国化学会第八届全国配位化学会议

作者： Jie-Luo Xue-Wen Wei di-chang zhong Yan-Chao Yang Ji-Hua Deng School of Chemistry & Chemical Engineering Gannan Normal University

With potential functions in molecular recognition,molecular catalysis,molecular transport and so on,the self-assembly of supramolecular architectures have received considerable attentions during the past several decades[1-2].Supramolecular architectures are usually stabilized by intermolecular noncovalent interactions including hydrogen bond,∏…∏ stacking interaction,hydrophobic interaction and so on[3-4].It is well-known that the characteristic and structure of the building block are key factors for constructions of functional supramolecular *** ideal building block generally possesses multi-interaction sites to bind with other molecules,and directs the crystal growth to get desired supramolecular networks.1,4-benzeneditetrazole(H

关键词： 1,4-benzeneditetrazole supramolecular compounds crystal structures crystalline materials

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