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CdTe/CdSe-sensitized photocathode coupling with Ni-substituted polyoxometalate catalyst for photoelectrochemical generation of hydrogen

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Nano Research 2022年第2期15卷 1347-1354页

作者： Junhao Zhang Mo Zhang Yuanyuan Dong Congcong Bai Yeqin Feng Le Jiao hongjin lv MOE Key Laboratory of Cluster Science School of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 102488China

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.

关键词： polyoxometalates quantum dots-sensitized photocathode favorable energetic gradient photoelectrochemical water splitting hydrogen generation

Recent advances of mixed-transition-metal-substituted polyoxometalates

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Science China Chemistry 2022年第8期65卷 1515-1525页

作者： Zhimin Wang Xing Xin Mo Zhang Zheng Li hongjin lv Guo-Yu Yang MOE Key Laboratory of Cluster Science Beijing Key Laboratory of Photoelectroic/Electrophotonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 102488China

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.

关键词： polyoxometalates lacunary POM ligands mixed-transition-metal substitution structural diversity catalysis

Atomically-precise Janus polyoxometalate catalyst with tunable water splitting activity

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Science China Chemistry 2023年第6期66卷 1771-1780页

作者： Zhimin Wang Xing Xin Zheng Li Mo Zhang Jiangwei Zhang Yeqin Feng Junhao Zhang hongjin lv Guo-Yu Yang MOE Key Laboratory of Cluster Science Beijing Key Laboratory of Photoelectroic/Electrophotonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 102488China College of Chemistry and Chemical Engineering Inner Mongolia UniversityHohhot 010021China

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.

关键词： Janus polyoxometalate catalyst mixed-transition-metal substitution X-ray absorption fine structure(XAFS) H evolution O evolution

Efficient Photogeneration of Hydrogen Boosted by Long-Lived Dye-Modified Ir(III)Photosensitizers and Polyoxometalate Catalyst

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CCS Chemistry 2022年第1期4卷 259-271页

作者： Lin Qin Chongyang Zhao Liao-Yuan Yao Hongbin Dou Mo Zhang Jing Xie Tsu-Chien Weng hongjin lv Guo-Yu Yang MOE Key Laboratory of Cluster Science School of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 102488 Department of Chemistry The University of Hong KongHong Kong 999077 School of Physical Science and Technology ShanghaiTec UniversityShanghai 201210

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.

关键词： dye-modified Ir(III)complexes Ni-substituted polyoxometalate visible-light-driven H_(2)evolution efficient intersystem crossing DFT calculations

Ring-Shaped Polyoxometalate Built by {Mn_(4)PW_(9)} and PO_(4) Units for Efficient Visible-Light-Driven Hydrogen Evolution

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CCS Chemistry 2021年第8期3卷 2095-2103页

作者： Hai-Lou Li Mo Zhang Chen Lian Zhong-Ling Lang hongjin lv Guo-Yu Yang MOE Key Laboratory of Cluster Science School of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 102488 MOE Key Laboratory of Polyoxometalate Science College of ChemistryNortheast Normal UniversityChangchunJilin 130024

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.

关键词： polyoxometalates polynuclear manganese clusters visible-light irradiation hydrogen evolution

轮型二十核铜取代多金属氧酸盐催化剂:光催化制氢的机理和稳定性研究

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Chinese Journal of Catalysis 2022年第2期43卷 442-450页

作者：冯业芹秦琳张峻豪符方玉李慧杰相华吕红金北京理工大学化学与化工学院原子分子簇科学教育部重点实验室北京102488

能源危机和环境污染已成为影响全人类的严峻问题,太阳能驱动水分解制备清洁可再生的氢能是解决以上问题的有效途径之一,因此,近年来环境友好的光驱动制氢方式受到广泛关注.现阶段太阳能驱动水分解体系的研究热点和难点在于研发高催化活... 详细信息

能源危机和环境污染已成为影响全人类的严峻问题,太阳能驱动水分解制备清洁可再生的氢能是解决以上问题的有效途径之一,因此,近年来环境友好的光驱动制氢方式受到广泛关注.现阶段太阳能驱动水分解体系的研究热点和难点在于研发高催化活性且廉价的非贵金属催化剂.作为具有较大应用潜力的多电子转移催化剂,廉价过渡金属取代的多金属氧酸盐因其合成策略丰富多样,原子结构明晰以及物化性质可调,越来越多地被用于催化水分解的研究中.其结构中的缺位多酸配体具有可逆的电子存储能力,因而可被用作多电子存储海绵,而过渡金属中心则可以作为催化活性位点,这种特殊的协同工作机制可有效促进催化反应中的电荷分离并延长电子的寿命,更利于催化还原反应的发生.虽然目前文献中有较多关于廉价3d过渡金属取代的多金属氧酸盐水还原催化剂的报道;然而,现阶段基于廉价过渡金属铜取代的多金属氧酸盐在光驱动分解水制氢领域的研究较少.这主要受制于理论计算得出的传统结论:氢原子在铜原子上的氢吸附吉布斯自由能比较高,可能会导致铜基催化剂具有比较低的产氢活性.本文合成了轮型二十核铜取代多金属氧酸盐水还原催化剂K_(12)Li_(13)[Cu_(2)0Cl(OH)_(24)(H_(2)O)_(12)(P_(8)W_(48)O_(184))]·22H_(2)O(K_(12)Li_(13)-Cu_(2)0P_(8)W_(48)),然后通过简单的阳离子交换制备了其四丁基铵盐(TBA-Cu_(2)0P_(8)W_(48)),红外表征结果表明,阳离子交换能够完整地保持其阴离子结构.利用[Ir(ppy)2(dtbbpy)][PF_(6)]作为光敏剂,三乙醇胺(TEOA)为牺牲试剂和TBA-Cu_(2)0P_(8)W_(48)为催化剂构筑光催化体系,反应5 h后产氢转化数达到~2892,120 h后高达~13400.此外,稳态和瞬态荧光猝灭光谱表明,激发态的光敏化剂既可以被TBA-Cu_(2)0P_(8)W_(48)氧化型猝灭,也可以被TEOA还原型猝灭,其中后者占主导.稳定性测试实验结果表明,在光催化过程中,TBA-Cu_(2)0P_(8)W_(48)分子催化剂上有Cu离子缓慢解离到反应溶液中,但其光催化产氢的主要催化活性物种仍具备分子催化剂的骨架结构.本文不仅对多核铜基分子化合物能够高效地催化光驱动产氢提供有利证明,而且为探索更多廉价铜取代多金属氧酸盐在太阳能转化领域的应用提供了参考.

关键词：多金属氧酸盐二十核铜取代光催化产氢光催化机理稳定性研究

过渡金属修饰{P2W12}基多酸化合物的研究进展

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中国科学：化学 2020年第9期50卷 1015-1030页

作者：辛兴吕红金北京理工大学化学与化工学院原子分子簇科学教育部重点实验室北京102488

多金属氧酸盐由于具有独特的结构组成与物理化学性质,如原子结构明晰、组成多样可控、得失电子/质子稳定可逆、丰富的氧化还原特性等,目前已成为无机化学中历史较为悠久、交叉渗透最广的研究领域之一.本文综述了多金属氧酸盐领域的重要... 详细信息

多金属氧酸盐由于具有独特的结构组成与物理化学性质,如原子结构明晰、组成多样可控、得失电子/质子稳定可逆、丰富的氧化还原特性等,目前已成为无机化学中历史较为悠久、交叉渗透最广的研究领域之一.本文综述了多金属氧酸盐领域的重要系列之一——过渡金属修饰{P2W12}基多酸化合物的研究进展,根据{P2W12}构筑模块的聚合数分类归纳了该系列化合物的相关结构,阐述了部分代表性化合物的结构特点及合成策略,整理了该类化合物的功能应用,并对其未来发展趋势进行了展望.

关键词：多金属氧酸盐过渡金属修饰 {P2W12}和{P8W48}构筑模块

异金属取代的多金属氧酸盐@光响应型金属-有机框架用于高选择性光催化CO_(2)还原

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Chinese Journal of Catalysis 2023年第7期50卷 343-351页

作者：李慧杰池漫洲辛兴王瑞杰刘天府吕红金杨国昱北京理工大学化学与化工学院光电/电光转换材料北京重点实验室原子分子簇科学教育部重点实验室北京102488

传统化石燃料的过度消耗以及CO_(2)的持续排放,使开发可再生的碳中性燃料迫在眉睫.利用太阳能将CO_(2)光还原为能量密集的有机分子(CO,HCOOH,HCHO和CH_(3)OH等)被认为是一种绿色可持续但极具挑战性的方案.实现该方案所面临的关键难点是... 详细信息

传统化石燃料的过度消耗以及CO_(2)的持续排放,使开发可再生的碳中性燃料迫在眉睫.利用太阳能将CO_(2)光还原为能量密集的有机分子(CO,HCOOH,HCHO和CH_(3)OH等)被认为是一种绿色可持续但极具挑战性的方案.实现该方案所面临的关键难点是开发高效、廉价的光催化CO_(2)还原催化剂.作为一种具有前景的多电子转移催化剂,过渡金属取代的多金属氧酸盐(POM)因其结构丰富且物化性质可调,越来越多地被应用于光催化CO_(2)还原研究.其结构中的缺位多酸配体可用作电子存储海绵以实现光催化CO_(2)还原反应中的多电子转移过程.然而,目前均相催化体系面临的主要挑战在于可溶性POMs催化剂的可回收性不高和催化活性低等.为解决上述挑战,可行的策略是将可溶性POMs催化剂装载到多孔金属有机框架(MOFs)中,制备POM@MOF复合材料,从而将可溶性POMs催化剂优越的催化活性与多孔材料的可回收性结合起来.作为一类光敏型MOF材料,NU-1000具有良好的光响应能力和合适的孔道结构,可容纳不同尺寸的POMs客体分子.目前,基于POM@NU-1000的复合材料在光驱动分解水制氢领域已有一些报道;然而,该类复合材料在太阳能驱动的光催化CO_(2)还原中的应用研究仍然较少.本文构筑了一种异金属取代的POM@NU-1000复合材料(P_(2)W_(15)Ni_(3){Re(CO)_(3)}_(3)@NU-1000)通过浸渍法将Ni-Re异金属取代POMs(Na(NH4)5[P_(2)W_(15)O_(56)Ni_(3)(H_(2)O)3(μ3-OH)3{Re(CO)3}3]·18H_(2)O)锚定到NU-1000MOF孔道中.系列实验实验证实了P_(2)W_(15)Ni_(3){Re(CO)_(3)}_(3)客体团簇成功装载进NU-1000主体的孔道中.在最佳条件下,P_(2)W_(15)Ni_(3){Re(CO)_(3)}_(3)@NU-1000复合材料能有效地进行光催化CO_(2)还原,反应10 h的CO产量高达28982μmolg^(–1),选择性达93.5%.此外,该催化体系具有良好的光催化稳定性和至少4次连续循环的可重复性.催化反应机理研究表明,高效的光催化CO_(2)还原性能归因于P_(2)W_(15)Ni_(3){Re(CO)_(3)}_(3)团簇独特的结构完整性、NU-1000优良的光响应能力以及二者之间强的主-客体相互作用.综上,本工作展示了引入CO_(2)还原功能单元到POMs客体分子的策略可调节POM@MOF功能复合材料的催化活性,为设计和合成高效率CO_(2)还原光催化剂提供了实验参考.

关键词： CO_(2)还原多金属氧酸盐金属有机框架材料异金属取代光催化

6%羟乙基淀粉130/0.4对创伤性家兔炎症介质及其信号通路的影响

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现代医药卫生 2023年第2期39卷 211-215,219页

作者：吕洪锦张倩黄绍艳张建中龙口市人民医院麻醉科山东烟台265700 滨州医学院第二临床医学院山东烟台264000 烟台市烟台山医院麻醉科山东烟台264000

目的探讨6%羟乙基淀粉(HES)130/0.4对创伤性家兔炎症介质及其信号通路——微小RNA(miR)-146a/Toll样受体-4(TLR4)/核因子-κB(NF-κB)的影响。方法 2022年4月选取新西兰雄性家兔16只,麻醉后用钝器敲打家兔的后肢造成后肢骨折,然后行骨... 详细信息

目的探讨6%羟乙基淀粉(HES)130/0.4对创伤性家兔炎症介质及其信号通路——微小RNA(miR)-146a/Toll样受体-4(TLR4)/核因子-κB(NF-κB)的影响。方法 2022年4月选取新西兰雄性家兔16只,麻醉后用钝器敲打家兔的后肢造成后肢骨折,然后行骨折切开内固定术。常规备皮、消毒,骨折部位外侧切口,显露股骨骨折部位,胯骨折线置入合适的国产四孔钢板,在骨折对应的肌肉组织2 cm×2 cm制作软组织缺损模型,同时,取血液和骨折部分肌肉组织备检(T_(0))。将家兔采用随机数字表法分为乳酸钠林格(LR)组和HES组,每组8只。LR组注射10 mL/kg LR,HES组注射10 mL/kg HES,每天1次,输注5 d,结束后将家兔麻醉取损伤部位肌肉组织备检(T_(1))。采用酶联免疫吸附试验法测定T_(0)、T_(1)时家兔血液肿瘤坏死因子-α(TNF-α)、白细胞介素-1(IL-1)、IL-6等,蛋白质印迹法测定T_(0)、T_(1)时家兔肌肉组织NF-κB P65、TLR4、IL-1受体相关激酶1(IRAK1)和TNF受体相关因子6(TRAF6)蛋白,逆转录-聚合酶链反应法检测T_(0)、T_(1)时家兔肌肉组织miR-146a。结果与T_(0)时比较,2组家兔T_(1)时血液TNF-α、IL-1、IL-6水平,以及肌肉miR-146a、NF-κB P65、TLR4、IRAK1、TRAF6蛋白水平均明显升高,差异均有统计学意义(P<0.05)。与LR组比较,HES组家兔T_(1)时血液TNF-α、IL-1、IL-6水平,以及肌肉组织NF-κB P65、TLR4、IRAK1、TRAF6蛋白水平均明显降低,肌肉组织miR-146a表达水平明显升高,差异均有统计学意义(P<0.05)。结论 HES可能通过上调miR-146a表达水平,负反馈调节TLR4信号通路上的IRAK1、TRAF6,抑制炎症介质的产生而减轻创伤家兔的炎性反应。

关键词：羟乙基淀粉微小RNA-146a Toll样受体4 NF-κB 兔炎性反应