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Residual solvent extraction via chemical displacement for efficient and stable perovskite solar cells

Journal of Energy Chemistry 2021年第10期30卷 8-14,I0001页

作者： Min Fang Lei Tao Wen Wu Qi Wei Yingdong Xia Ping Li Xueqin Ran Qi Zhong Guichuan Xing Lin Song Peter Müller-Buschbaum Hui Zhang Yonghua Chen Key Laboratory of Flexible Electronics(KLOFE)&Institution of Advanced Materials(IAM) Nanjing Tech University(Nanjing Tech)Nanjing 211816JiangsuChina Frontiers Science Center for Flexible Electronics Xi’an Institute of Flexible Electronics(IFE)and Xi’an Institute of Biomedical Materials&EngineeringNorthwestern Polytechnical UniversityXi’an 710072ShaanxiChina Key Laboratory of Advanced Textile Materials&Manufacturing Technology Ministry of EducationZhejiang Sci-Tech UniversityHangzhou 310018ZhejiangChina Institute of Joint Key Laboratory of the Applied Physics and Materials Engineering University of MacaoAvenida da UniversidadeTaipa 999078MacaoChina Lehrstuhl für Funktionelle Materialien Physik DepartmentTechnische Universität München.James-Franck-Str.185748 GarchingGermany Heinz Maier-Leibnitz Zentrum(MLZ) Technische Universität MünchenLichtenbergstr.185748 GarchingGermany

Solvent residue is inevitable to occur in solution processed thin films,but its influence on the thin film quality has not been identified and addressed to *** acetate(MAAc)ionic liquid has recently been realized as an environmentally friendly solvent for solution processed *** specific high viscosity,low vapor pressure and strong association with perovskite precursor of the MAAc solvent is a double-edged sword,which endowed an advantageously ambient air operational and anti-solvent free perovskite deposition,but the MAAc is likely to be retained within the film and bring in detrimental effects on device performance of the corresponding solar ***,we reported a novel route to eliminate the residual solvent via a facial hydrochloric acid(HCl)annealing post-treatment(HAAP).In particular,chemical displacement reaction between the incorporated HCl and residual MAAc can be initiated to form volatile MACl and HAc,efficiently extracting MAAc *** the meanwhile,the stimulated mass transport via downward penetration and upward escape can trigger secondary perovskite growth with enlarged grain size and smoothened surface,leading to reduced defect state and improved interfacial contact intimacy,and also partial chloride ions are able to enter the crystal lattice to stabilize perovskite phase *** a result,a champion efficiency up to20.78%originating from enhanced Voc was achieved,and more than 96%of its initial efficiency can be maintained after 1000 h shelf-storage.

关键词： Perovskite Solar cells Solvent residue Methylammonium acetate Post-treatment Chemical displacement

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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 *** 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 ***,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 *** 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 *** 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

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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 *** 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 *** 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 ***,a comprehensive outlook of this research area was also prospected.

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

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Polyoxometalate-organic cage with{Ni_(4)SiW_(9)}node for photocatalytic hydrogen evolution

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Chinese Chemical Letters 2024年第3期35卷 177-181页

作者： Jing Li Yeqin Feng Fangyu Fu Xing Xin Guoyu Yang Hongjin Lv MOE Key Laboratory of Cluster Science Beijing Key Laboratory of Photoelectroic/Electrophotonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 102488China

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 *** 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 *** 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 *** 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 *** 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.

关键词： Polyoxometalate Polyoxometalate-organic cages Photocatalytic hydrogen production Visible light illumination

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Copper-catalyzed decarboxylative hydroboration of phenylpropiolic acids under ligand-free or both ligand-and base-free conditions

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Chinese Chemical Letters 2016年第4期27卷 571-574页

作者： Ying-Wei Zhao Qiang Feng Qiu-Ling Song Institute of Next Generation Matter Transformation College of Chemical Engineering Huaqiao University

An efficient copper-catalyzed decarboxylative hydroboration of phenylpropiolic acids with bis（pinacolato）diboron was developed, affording b-vinylboronates as the only products in high yields. Extra hydrogen sources such as methanol are not needed in this catalytic system. This reaction could be performed successfully under ligand- and base-free conditions. It demonstrated that phenylpropiolic acids can be employed as alkyne synthons in the hydroboration reaction and exhibited good reactivity and higher selectivity than terminal alkynes.

关键词： Decarboxylation Hydroboration Ligand-free Base-free Copper-catalysis

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Origin of High Efficiency and Long-Term Stability in Ionic Liquid Perovskite Photovoltaic

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Research 2020年第1期2020卷 391-403页

作者： Lingfeng Chao Tingting Niu Hao Gu Yingguo Yang Qi Wei Yingdong Xia Wei Hui Shouwei Zuo Zhaohua Zhu Chengjie Pei Xiaodong Li Jing Zhang Junfeng Fang Guichuan Xing Hai Li Xiao Huang Xingyu Gao Chenxin Ran Lin Song Li Fu Yonghua Chen Wei Huang Frontiers Science Center for Flexible Electronics Xi’an Institute of Flexible Electronics(IFE)and Xi’an Institute of Biomedical Materials&EngineeringNorthwestern Polytechnical University127 West Youyi RoadXi’an 710072China Key Laboratory of Flexible Electronics(KLOFE)&Institution of Advanced Materials(IAM) Nanjing Tech University(Nanjing Tech)Nanjing211816 JiangsuChina Shanghai Synchrotron Radiation Facility Shanghai Institute of Applied PhysicsChinese Academy of SciencesShanghai 201204China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China School of Physics and Electronic Science Ministry of EducationNanophotonics&Advanced Instrument Engineering Research CenterEast China Normal UniversityShanghai 200062China Institute of Applied Physics and Materials Engineering University of MacaoMacaoMacao SAR 999078China Key Laboratory for Organic Electronics&Information Displays(KLOEID)and Institute of Advanced Materials(IAM) Nanjing University of Posts and TelecommunicationsNanjing210023 JiangsuChina

Environment-friendly protic amine carboxylic acid ionic liquids(ILs)as solvents is a significant breakthrough with respect to traditional highly coordinating and toxic solvents in achieving efficient and stable perovskite solar cells(PSCs)with a simple one-step air processing and without an antisolvent treatment ***,it remains mysterious for the improved efficiency and stability of PSCs without any passivation ***,we unambiguously demonstrate that the three functions of solvents,additive,and passivation are present for protic amine carboxylic acid *** found that the ILs have the capability to dissolve a series of perovskite precursors,induce oriented crystallization,and chemically passivate the grain *** is attributed to the unique molecular structure of ILs with carbonyl and amine groups,allowing for strong interaction with perovskite precursors by forming C=O…Pb chelate bonds and N-H…I hydrogen bonds in both solution and *** finding is generic in nature with extension to a wide range of IL-based perovskite optoelectronics.

关键词： perovskite bonds breakthrough

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Recent advances in the syntheses of pyrroles

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Green Synthesis and Catalysis 2023年第1期4卷 20-34页

作者： Tao Shi Gaofeng Yin Xiaodong Wang Yongxia Xiong Yan Peng Shuang Li Yaofu Zeng Zhen Wang School of Pharmacy Lanzhou UniversityLanzhou 730000China School of Pharmaceutical Science Hengyang Medical SchoolUniversity of South ChinaChangsha 421001China

The pyrrole moiety is an important structural motif in functional materials,natural products,and *** and more synthetic strategies toward pyrroles have emerged,where various efficient building blocks are developed and these synthons enable the syntheses of pyrroles with different numbers of ***,no review specifically summarizes the syntheses of pyrroles according to the type and number of employed building *** aid researchers to design appropriate substrates for pyrrole synthesis,herein we summarized the advances in pyrrole syntheses and classified these reactions into four categories according to the number of employed components,which may shed light on developing more efficient synthetic methods toward substituted pyrroles.

关键词： Pyrrole Mono-component strategies Two-component strategies Three-component strategies Four-component strategies Multi-component reactions

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A universal ionic liquid solvent for non-halide lead sources in perovskite solar cells

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Journal of Energy Chemistry 2022年第8期31卷 445-451,I0012页

作者： Yue Chen Yamin Xu Jin Liu Yuexin Lin Jianfei Hu Chensi Cao Yingdong Xia Yonghua Chen Key Laboratory of Flexible Electronics(KLOFE)and Institute of Advanced Materials(IAM) Nanjing Tech UniversityNanjing 211816JiangsuChina

Replacing lead iodide(PbI_(2))with suitable non-halides lead source has been found to be an effective method to control crystallization and fabricate high-performance perovskite solar cells(PSCs).However,the solubility of non-halide lead sources is highly limited by traditional solvents due to the chemical interaction ***,we report a series of non-halide lead sources(e.g.,lead acetate(PbAc_(2)),lead sulfate(PbSO_(4)),lead carbonate(PbCO_(3)),lead nitrate(Pb(NO_(3))_(2)),lead formate(Pb(HCOO)_(2))and lead oxalate(PbC_(2)O_(4)))can be well dissolved in an ionic liquid solvent methylammonium acetate(MAAc).We found that the universal strong coordination of C=O with lead ion(Pb^(2+))and the formation of hydrogen bonds were observed in perovskite precursor *** allows the dissolution of non-halide lead salts and is able to produce perovskite film with smooth,compact,and full coverage crystal *** power conversion efficiency(PCE)of 14.48%,19.21%,and 20.13%in PSCs based on PbSO_(4),PbAc_(2),and PbCO_(3) was achieved,respectively,in the absence of any additives and passivation *** study demonstrates the universality of ionic liquid for the preparation of PSCs based on nonhalides lead sources.

关键词： Efficiency Non-halide lead Precursor components Perovskite solar cells Universality

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Immobilizing polysulfide jointly via chemical absorbing and physical blocking in polytungstates-embedded carbon nanofibers

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Journal of Energy Chemistry 2021年第6期30卷 206-211,I0006页

作者： Yanmei Nie Lei Tan Guangchao Li Sanghao Li Jun Yan Jiexi Wang College of Chemistry and Chemical Engineering&School of Metallurgy and Environment Central South UniversityChangsha 410083HunanChina Hunan Provincial Key Laboratory of Chemical Power Sources Central South UniversityChangsha 410083HunanChina Engineering Research Center of the Ministry of Education for Advanced Battery Materials Central South UniversityChangsha 410083HunanChina

Lithium-sulfur(Li-S) battery is regarded as one of the most fascinating candidates for energy storage due to its dominant advantage of high energy ***,the shuttling effect of soluble polysulfides and low electrical conductivity of sulfur and Li_(2)S still hinder its *** this work,high electrical-conductive carbon nanofibers(CNFs) with uniformly embedded polytungstates(HPW@CNFs) are proposed for advanced Li-S batteries.H_(3)PW_(12)O_(40)(HPW) is a kind of molecular nano-sized metal cluster which contains rich Lewis acid/base sites that can stabilize polysulfide effectively through chemical bonding,while CNFs play the role of physical barriers for polysulfides and transmission channel for *** HPW@CNFs/S cathode shows an ultra-stable cycling performance with extremely small decay rate of 0.015% per cycle over 400 cycles at 0.5 C.

关键词： Lithium-sulfur batteries Polysulfides Polyoxometalates Carbon nanofibers

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Solution processed nano-ZnMgO interfacial layer for highly efficient inverted perovskite solar cells

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Journal of Energy Chemistry 2019年第1期28卷 107-110页

作者： Ze Wang Yingdong Xia Lingfeng Chao Yufeng Pan Meijin Li Renzhi Li Bin Du Yonghua Chen Wei Huang Key Laboratory of Flexible Electronics (KLOFE) & Institution of Advanced Materials (IAM) Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM) Nanjing Tech University (NJTECH) Shaanxi Institute of Flexible Electronics (SIFE) Northwestern Polytechnical University (NPU) Key Laboratory for Organic Electronics & Information Displays (KLOEID) and Institute of Advanced Materials (IAM) Nanjing University of Posts and Telecommunications

Interfacial layer has a significant impact on the achievement of highly efficient organic–inorganic hybrid perovskite solar cells(PSCs). Here, we introduced a nano-ZnMgO(magnesium doped ZnO, abbreviated as ZnMgO) as interfacial layer between [6, 6]-Phenyl C_(61) butyric acid methyl ester(PC_(61) BM) layer and Al electrode to replace LiF or ZnO interlayer and enhance device performance. The device efficiency has been improved from 11.43% to 15.61% and the hysteresis was decreased dramatically. Such huge enhancement of power convert efficiency(PCE) can be attributed to the low dark current density, enhancement of electron-selective contact, and low energy barrier at the PC_(61) BM/Al interface. We suggest that this simple nano-scale interlayer can provide an efficient charge transport and extraction for highly efficient PSCs.

关键词： Nano-ZnMgO Interfacial layer High efficiency Perovskite solar cells

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