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| 1 | Efficient Photogeneration of Hydrogen Boosted by Long-Lived Dye-Modified Ir(III)Photosensitizers and Polyoxometalate Catalyst显示文摘Developing efficient catalysts and photosensitizers is crucial for the construction of effective photocatalytic H2-evolving systems.Here,we report the facile preparation of Coumarin-modified Ir(III)complexes(PS-2 and PS-3)and their utilization as chromophores to drive favorable photocatalytic H2 evolution using Ni-substituted polyoxometalate(Ni_(3)PW_(10))catalyst and triethanolamine(TEOA)as an electron donor.Compared with the commercially available unmodified Ir(III)complex(PS-1),both PS-2 and PS-3 displayed intensive absorption in the range of 400–550 nm with ε_(max) of 110,620 and 91,430 M^(−1) cm6(−1),respectively.Varying the substitutes on the bipyridine ligand affected their physicochemical properties and the corresponding photocatalytic activity dramatically.Under photocatalytic conditions,the quantity of H2 molecules generated by PS-2-and PS-3-containing systems were 13.1 and 2.1 times,respectively,that of the PS-1-containing system.When PS-2 was used as a photosensitizer,the highest turnover number(TON)of 19,739 was obtained versus Ni_(3)PW_(10) catalyst.Various spectroscopic and computational studies have revealed that factors such as strong and broad visible-light-absorbing ability,long-lived triplet state,suitable redox potential,opposed by using polyoxometalate(POM)catalyst,and large highest occupied molecular orbital(HOMO)–lowest unoccupied molecular orbital(LUMO)gap of PS-2 attributed to drastically enhanced photocatalytic activity. | Lin Qin Chongyang Zhao Liao-Yuan Yao Hongbin Dou Mo Zhang Jing Xie Tsu-Chien Weng Hongjin Lv Guo-Yu Yang | 2022 | CCS Chemistry2022，4，1： | 1 |
| 2 | Ring-Shaped Polyoxometalate Built by {Mn_(4)PW_(9)} and PO_(4) Units for Efficient Visible-Light-Driven Hydrogen Evolution显示文摘A novel mixed-valence,ring-shaped multinuclear Mn-containing polyoxometalate,[H_(2)N(CH_(3))_(2)]_(15) NaH8-[Mn^(Ⅲ) 3MnIV(μ3-O)_(3)(OAc)PO4(B-α-PW_(9)O_(34))]_(4)·36H_(2)O(1)was made and systematically characterized using various spectroscopic and computational techniques.Its polyoxoanion can be described as a tetramer made of four[Mn^(Ⅲ) 3MnIV(μ3-O)3(OAc)(B-α-PW_(9)O_(34))]_(3)−({Mn^(Ⅲ) 3Mn^(IV)(PW_(9))})clusters and four PO_(4) linkers. | Hai-Lou Li Mo Zhang Chen Lian Zhong-Ling Lang Hongjin Lv Guo-Yu Yang | 2021 | CCS Chemistry2021，3，8： | 1 |
| 3 | Recent advances of mixed-transition-metal-substituted polyoxometalates显示文摘Polyoxometalates(POMs)have been emerging as one of the most widely-studied interdisciplinary research fields of inorganic chemistry due to their structural diversities and versatile physicochemical properties.The incorporation of transition metals into lacunary POM ligands can lead to the formation of various transition-metal-substituted POMs(TMSPs)with wide potential applications in research areas including medicine,magnetism,functional materials,catalysis,and energy storage.In this review,we summarized the recent advances of mixed-transition-metal-substituted POMs(Mixed TMSPs)with respect to their synthetic strategies,structural diversities,and relevant applications.Finally,a comprehensive outlook of this research area was also prospected. | Zhimin Wang Xing Xin Mo Zhang Zheng Li Hongjin Lv Guo-Yu Yang | 2022 | Science China Chemistry2022，65，8： | 1 |
| 4 | Hole removal rate limits photodriven H2 generation efficiency in CdS- Pt and CdSe/CdS-Pt semiconductor nanorod+metal Tip heterostructures 显示文摘 | WU Kaifeng CHEN Zheyuan LV Hongjin | 2014 | J Am Chem Soc2014，136，21： | 1 |
| 5 | Atomically-precise Janus polyoxometalate catalyst with tunable water splitting activity显示文摘The development of bifunctional catalysts for solar-driven hydrogen and oxygen evolution has been regarded as a challenging but interesting research topic.As promising multi-electron-transfer catalysts,previously reported polyoxometalate(POM)-based catalysts often contain only a single type of transition metal substitution for driving either hydrogen production or oxygen evolution.Herein,a viable two-step parental substitution approach has been developed to synthesize two structurally-new mixed-transition-metal-substituted polyoxometalates(mixed TMSPs),K_(6)Na_(4)[Mn_(2)Ni_(2)(H_(2)O)2(PW_(9)O_(34))2]·21H_(2)O({Mn_(2)Ni_(2)})and K10[Mn_(2)Co_(2)(H_(2)O)2(PW_(9)O_(34))2]·35H_(2)O({Mn_(2)Co_(2)}),using Na_(12)[Mn_(2)Na_(2)(PW_(9)O_(34))2]·36H_(2)O({Mn_(2)Na_(2)})as the precursor.Characterization results confirmed the nearly quantitative substitution of Na+with Ni_(2)+and Co_(2+)ions.X-ray absorption fine structure(XAFS)spectroscopy revealed that the Mn atoms are preferentially located in the internal positions of the central belt while Ni and Co atoms preferentially reside in the external,solvent-accessible positions.Benefiting from the second substitution of catalytically active transition metals,the resulting{Mn_(2)Ni_(2)}and{Mn_(2)Co_(2)}can be utilized as Janus catalysts towards H_(2) evolution and O_(2) evolution under visible light irradiation with greatly-enhanced activity compared to that of parental{Mn_(2)Na_(2)}.The introduction of mixed transition metals into POM structures not only enriches the POMs family,but also provides an effective strategy to control electronic structures and catalytic properties of POM-based catalysts at the atomic level. | Zhimin Wang Xing Xin Zheng Li Mo Zhang Jiangwei Zhang Yeqin Feng Junhao Zhang Hongjin Lv Guo-Yu Yang | 2023 | Science China Chemistry2023，66，6： | 0 |
| 6 | Polyoxometalate-organic cage with{Ni_(4)SiW_(9)}node for photocatalytic hydrogen evolution显示文摘The design and syntheses of metal-organic cages(MOCs)based on polyoxometalates(POMs)building blocks have attracted increasing attention due to their intriguing molecular architectures and physicochemical properties.In this work,we have successfully synthesized and systematically characterized a tetrahedral polyoxometalate-based organic cage(POC),K_(3)Na_(17)H_(12)[(C_(4)H_(6)O_(6))_(6)[Ni_(4)(OH)_(3)(A-α-SiW_(9)O_(34))]_(4)]·96H_(2)O(Ni_(16)L_(6)(SiW_(9))_(4)),using tritopic Ni_(4)-substituted Keggin cluster(Ni_(4)SiW_(9))as nodes and flexible L-(+)-tartaric acid ligands as linkers.The resulting POC tetrahedron has been firstly investigated as efficient catalyst for visible-light-driven hydrogen production,achieving a turnover number of 15,500 after 96-h photocatalysis.Such high catalytic performance of Ni_(16)L_(6)(SiW_(9))_(4)POC catalyst could be attributed to its unique cage structure,thereby offering more efficient catalytic component accessibility.In addition,spectroscopic analyses illustrated the photocatalytic mechanism and the structural stability of the TBA-Ni_(16)L_(6)(SiW_(9))_(4)catalyst during the photocatalytic process. | Jing Li Yeqin Feng Fangyu Fu Xing Xin Guoyu Yang Hongjin Lv | 2024 | Chinese Chemical Letters2024，35，3： | 0 |
| 7 | CdTe/CdSe-sensitized photocathode coupling with Ni-substituted polyoxometalate catalyst for photoelectrochemical generation of hydrogen显示文摘In terms of photoelectrochemical(PEC)hydrogen evolution,substantial challenge still remains regarding the controllable fabrication of quantum dots(QDs)-sensitized photocathodes with enhanced visible-light absorption,efficient charge carrier separation,and directional migration at the electrode interface.In this work,the CdTe/CdSe QDs-sensitized photocathodes were delicately constructed on p-type NiO-coated indium tin oxide(ITO)electrodes by spin-coating approach.The resulting co-sensitized photocathode exhibits a favorable pseudo-Type Ⅱ energetic band alignment that combines the advantages of strong light absorption of constituent QDs as well as the effective and oriented charge separation and migration.Upon green LED light illumination,the photogenerated electrons could be effectively transferred to a tetra-nickel-substituted polyoxometalate catalyst for hydrogen production while photogenerated holes will be scavenged at the NiO/ITO electrode.Under minimally optimized conditions,the pseudo-Type Ⅱ CdTe/CdSe-sensrtized photocathode yields a photcx:urrent density of over 100 pA/cm^(2) and a Faradaic efficiency of〜100%,which is among one of the most efficient QDs-based photocathode systems coupling with Ni-substituted polyoxometalate catalyst for photoelectrochemical hydrogen generation. | Junhao Zhang Mo Zhang Yuanyuan Dong Congcong Bai Yeqin Feng Le Jiao Hongjin Lv | 2022 | Nano Research2022，15，2： | 0 |
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