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A-site assisted perovskite crystallization via ion-exchange MOFs for high efficient and stable perovskite solar cells

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Journal of energy Chemistry 2024年第6期93卷 436-442,I0011页

作者： Xingrui Zhang Jian Zhang Wei Wang Boyuan Hu Yayu Dong Debin Xia Kaifeng Lin Yulin Yang miit key laboratory of Critical materials technology for new energy conversion and storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001HeilongjiangChina

Here,a novel strategy is proposed targeting the volatility of A-site cations and the disordered arrangement of perovskite grains through employing Cs~+contained metal-organic frameworks In-aip(Cs)obtained by ion-exchange and crystalline transform.Interatomic forces between Cs-O atoms split the pore channels of the pristine In-aip,endowing In-aip(Cs)with multidimensional charge transport channels,In addition,the partially freed Cs~+in the interlayer compensates for the vacancy of A-site cations during the perovskite preparation process.The In-aip(Cs)modified perovskite films have a flat morphology,large grains and excellent optoelectronic properties.Benefiting from the high-quality perovskite films and faster charge extraction,the In-aip(Cs)-modified PSCs achieved a champion PCE of 23.03%,superior to the In-aip-modified(22.29%)and control device(21.13%),More importantly,the unencapsulated PSCs modified with In-aip(Cs)exhibited outstanding humidity and thermal stability.Over a period of almost 1000 h,the unencapsulated In-aip(Cs)-modified device retained 85%of its initial PCE after storing in a glove box at 85℃,and retained 87%of the primary PCE upon storage in ambient condition at 25℃under a humidity of 40%.

关键词： Metal-organic frameworks PSCs Stability Defect passivation

Enhanced Redox Electrocatalysis in High‑Entropy Perovskite Fluorides by Tailoring d–p Hybridization

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Nano-Micro Letters 2024年第3期16卷 333-350页

作者： Xudong Li Zhuomin Qiang Guokang Han Shuyun Guan Yang Zhao Shuaifeng Lou Yongming Zhu Department of Applied Chemistry Harbin Institute of Technology at WeihaiWeihai 264209People’s Republic of China miit key laboratory of Critical materials technology for new energy conversion and storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001People’s Republic of China

High-entropy catalysts featuring exceptional properties are,in no doubt,playing an increasingly significant role in aprotic lithium-oxygen batteries.Despite extensive effort devoted to tracing the origin of their unparalleled performance,the relationships between multiple active sites and reaction intermediates are still obscure.Here,enlightened by theoretical screening,we tailor a high-entropy perovskite fluoride(KCoMnNiMgZnF_(3)-HEC)with various active sites to overcome the limitations of conventional catalysts in redox process.The entropy effect modulates the d-band center and d orbital occupancy of active centers,which optimizes the d–p hybridization between catalytic sites and key intermediates,enabling a moderate adsorption of LiO_(2)and thus reinforcing the reaction kinetics.As a result,the Li–O2 battery with KCoMnNiMgZnF_(3)-HEC catalyst delivers a minimal discharge/charge polarization and long-term cycle stability,preceding majority of traditional catalysts reported.These encouraging results provide inspiring insights into the electron manipulation and d orbital structure optimization for advanced electrocatalyst.

关键词： Lithium-oxygen batteries KCoMnNiMgZnF_(3)-HEC perovskite fluoride Entropy effect Catalytic kinetics d-p orbital hybridization

Recent progress in lanthanide ions doped inorganic metal halide perovskites

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Journal of Rare Earths 2024年第2期42卷 237-250,I0001页

作者： Yiyan Zhang Tianyu Zhao Guanying Chen miit key laboratory of Critical materials technology for new energy conversion and storage School of Chemistry and Chemical EngineeringState Key Laboratory of Urban Water Resource and EnvironmentKey Laboratory of Micro-systems and Micro-structuresMinistry of EducationHarbin Institute of TechnologyHarbin150001China

Benefiting from their large molar extinction coefficient,high carrier mobility,narrow and tunable emissions,inorganic metal halide perovskites(IMHPs) demonstrate great potential in various optoelectrical devices including solar cells,light emitting diodes and photodetectors in the past few years.Metal ions doping,well-known as a modification method of semiconductors,has been extensively applied in IMHPs as well.Diverse metal ions have been doped in IMHPs including alkali metals,alkali earth metals,transition metals and lanthanide metals,which either improve their optical performances or induce intriguing brand-new properties.Among them,lanthanide metals feature plentiful energy levels and stable optical properties and are one of the most noteworthy species.Here we review recent progress in lanthanide ions doped IMHPs.We summarize Yb,Eu or Er ions singly doping in detail,which was the most investigated species in IMHPs.Other lanthanide ions are also reviewed synoptically.Furthermore,we introduce lanthanide ions multi-doped IMHPs and at last we put forward several potential development directions.As the interests in lanthanide ions doped IMHPs rise,researchers have made some achievements in the field.Still though,there are more unexplored issues.Although there are review articles focusing on metal ions doped IMHPs or lanthanide ions doped perovskites,this review aims to provide an overall introduction of lanthanide ions doped IMHPs.This review may help researchers learn about lanthanide ions doped IMHPs and is to inspire researchers to make further promotion in this field.

关键词： Halide perovskite Lanthanide Doping Rare earths

Compositional and Hollow Engineering of Silicon Carbide/Carbon Microspheres as High-Performance Microwave Absorbing materials with Good Environmental Tolerance

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Nano-Micro Letters 2024年第9期16卷 128-146页

作者： Lixue Gai Yahui Wang Pan Wan Shuping Yu Yongzheng Chen Xijiang Han Ping Xu Yunchen Du miit key laboratory of Critical materials technology for new energy conversion and storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001People’s Republic of China Anhui Provincial laboratory of Advanced Laser technology College of Electronic EngineeringNational University of Defense TechnologyHefei 230037People’s Republic of China

Microwave absorbing materials(MAMs)characterized by high absorption efficiency and good environmental tolerance are highly desirable in practical applications.Both silicon carbide and carbon are considered as stable MAMs under some rigorous conditions,while their composites still fail to produce satisfactory microwave absorption performance regardless of the improvements as compared with the individuals.Herein,we have successfully implemented compositional and structural engineering to fabricate hollow SiC/C microspheres with controllable composition.The simultaneous modulation on dielectric properties and impedance matching can be easily achieved as the change in the composition of these composites.The formation of hollow structure not only favors lightweight feature,but also generates considerable contribution to microwave attenuation capacity.With the synergistic effect of composition and structure,the optimized SiC/C composite exhibits excellent performance,whose the strongest reflection loss intensity and broadest effective absorption reach−60.8 dB and 5.1 GHz,respectively,and its microwave absorption properties are actually superior to those of most SiC/C composites in previous studies.In addition,the stability tests of microwave absorption capacity after exposure to harsh conditions and Radar Cross Section simulation data demonstrate that hollow SiC/C microspheres from compositional and structural optimization have a bright prospect in practical applications.

关键词： SiC/C composites Compositional engineering Hollow engineering Microwave absorption Environmental tolerance

High donor-number and low content electrolyte additive for stabilizing zinc metal anode

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Journal of energy Chemistry 2024年第8期95卷 626-635页

作者： Yuxin Gong Ruifan Lin Bo Wang Huaizheng Ren Lei Wang Han Zhang Jianxin Wang Deyu Li Yueping Xiong Dianlong Wang Huakun Liu Shixue Dou miit key laboratory of Critical materials technology for new energy conversion and storage State Key Laboratory of Urban Water Resource and Environment School of Chemistry and Chemical Engineering Harbin Institute of Technology key laboratory of Advanced energy materials Chemistry(Ministry of Education) College of Chemistry Nankai University Institute of energy Material Science University of Shanghai for Science and Technology

The aqueous zinc ion batteries（AZIBs） are thought as promising competitors for electrochemical energy storage,though their wide application is curbed by the uncontrollable dendrite growth and gas evolution side reactions.Herein,to stabilize both zinc anodes and water molecules,we developed a modified electrolyte by adding a trace amount of N,N-diethylformanmide（DEF） into the ZnSO4electrolyte for the first time in zinc ion batteries.The effectiveness of DEF is predicted by the comparison of donor number and its preferential adsorption behavior on the zinc anode is further demonstrated by several spectroscopy characterizations,electrochemical methods,and molecular dynamics simulation.The modified electrolyte with 5% v.t.DEF content can ensure a stable cycling life longer than 3400 h of Zn‖Zn symmetric cells and an ultra-reversible Zn stripping/plating process with a high coulombic efficiency of 99.7%.The Zn‖VO2full cell maintains a capacity retention of 83.5% and a 104 mA h g-1mass capacity after 1000cycles.This work provides insights into the role of interfacial adsorption behavior and the donor number of additive molecules in designing low-content and effective aqueous electrolytes.

关键词： Aqueous zinc ion batteries Donor number Electrolyte additives Zinc anode Zinc dendrites

High-speed flexible near-infrared organic photodiode for optical communication

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National Science Review 2024年第3期11卷 227-238页

作者： Yu Zhu Hongbin Chen Ruiman Han Hao Qin Zhaoyang Yao Hang Liu Yanfeng Ma Xiangjian Wan Guanghui Li Yongsheng Chen The Centre of Nanoscale Science and technology and key laboratory of Functional Polymer materials Institute of Polymer ChemistryTianjin Key Laboratory of Functional Polymer Materials College of Chemistry and Renewable Energy Conversion and Storage Center(RECAST) Nankai University State key laboratory of Elemento-Organic Chemistry Nankai University

Optical communication is a particularly compelling technology for tackling the speed and capacity bottlenecks in data communication in modern society. Currently, the silicon photodetector plays a dominant role in high-speed optical communication across the visible-near-infrared spectrum. However, its intrinsic rigid structure, high working bias and low responsivity essentially limit its application in next-generation flexible optoelectronic devices. Herein, we report a narrow-bandgap non-fullerene acceptor（NFA） with a remarkable π-extension in the direction of both central and end units（CH17） with respect to the Y6 series, which demonstrates a more effective and compact 3D molecular packing, leading to lower trap states and energetic disorders in the photoactive film. Consequently, the optimized solution-processed organic photodetector（OPD） with CH17 exhibits a remarkable response time of 91 ns（λ = 880 nm） due to the high charge mobility and low parasitic capacitance, exceeding the values of most commercial Si photodiodes and all NFA-based OPDs operating in self-powered mode. More significantly, the flexible OPD exhibits negligible performance attenuation（<1%） after bending for 500 cycles, and maintains 96% of its initial performance even after 550 h of indoor exposure. Furthermore, the high-speed OPD demonstrates a high data transmission rate of 80 MHz with a bit error rate of 3.5 × 10-4, meaning it has great potential in next-generation high-speed flexible optical communication systems.

关键词： flexible organic photodetector high-speed NIR organic photodetector optical communication light fidelity narrow-bandgap non-fullerene acceptors

Photo-enhanced uranium recovery from spent fuel reprocessing wastewater via S-scheme 2D/0D C_(3)N_(5)/Fe_(2)O_(3) heterojunctions

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SusMat 2024年第2期4卷 41-50页

作者： Qi Meng Linzhen Wu Xiaoyong Yang Ying Xiong Fanpeng Kong Tao Duan State key laboratory of Environment-friendly energy materials NuclearWaste and Environmental Safety Key Laboratory of DefenseSouthwest University of Science and TechnologyMianyangSichuanChina miit key laboratory of Critical materials technology for new energy conversion and storage Harbin Institute of TechnologyHarbinHeilongjiangChina Department of materials Science and Engineering KTH Royal Institute of TechnologyStockholmSweden

Re-extracting environmentally transportable hexavalent uranium from wastew-ater produced by spent fuel reprocessing using the photocatalytic technology is a crucial strategy to avoid uranium pollution and recover nuclear fuel strategic resources.Here,we have designed S-scheme 2D/0D C_(3)N_(5)/Fe_(2)O_(3)heterojunction photocatalysts based on the built-in electric field and the energy band bend-ing theory,and have further revealed the immobilization process of hexavalent uranium conversion into relatively insoluble tetravalent uranium in terms of thermodynamics and kinetics.According to the results,the hexavalent uranium removal and recovery ratios in wastewater are as high as 93.38%and 83.58%,respectively.Besides,C_(3)N_(5)/Fe_(2)O_(3)heterojunctions also exhibit satisfactory cat-alytic activity and selectivity even in the presence of excessive impurity cations(including Na^(+),K^(+),Ca^(^(2+)),Mg^(2+),Sr^(2+),and Eu^(3+))or various organics(such as xylene,tributylphosphate,pyridine,tannic acid,citric acid,and oxalic acid).It is believed that this work can provide a potential opportunity for S-scheme heterojunction photocatalysts to re-enrich uranium from spent fuel wastewater.

关键词： nuclear wastewater S-scheme heterostructure uranium recovery

Solid-state synthesis and ion transport characteristics of theβ-KSbF_(4)for all-solid-state fluoride-ion batteries

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Journal of energy Chemistry 2024年第7期94卷 758-767页

作者： Jiali Liu Huahui Zhao Jingcheng Xia Lingguang Yi Xiaoyi Chen Dongdu Li Shuhan Ni Xinyi Su Yixuan Chen Min Liu Xianyou Wang National Base for International Science&technology Cooperation National Local Joint Engineering Laboratory for Key Materials of New Energy Storage BatteryHunan Province Key Laboratory of Electrochemical Energy Storage&ConversionSchool of ChemistryXiangtan UniversityXiangtan 411105HunanChina College of new energy Ningbo University of TechnologyNingbo 315336ZhejiangChina

All-solid-state fluoride ion batteries(FIBs)have been recently considered as a post-lithium-ion battery system due to their high safety and high energy density.Just like all solid-state lithium batteries,the key to the development of FIBs lies in room-temperature electrolytes with high ionic conductivity.β-KSbF_(4)is a kind of promising solid-state electrolyte for FIBs owing to its rational ionic conductivity and relatively wide electrochemical stability window at room temperature.However,the previous synthesis routes ofβ-KSbF_(4)required the use of highly toxic hydrofluoric acid and the ionic conductivity of as-prepared product needs to be further improved.Herein,the β-KSbF_(4)sample with an ionic conductivity of 1.04×10^(-4)s cm^(-1)(30°C)is synthesized through the simple solid-state route.In order to account for the high ionic conductivity of the as-synthesizedβ-KSbF_(4),X-ray diffraction(XRD),scanning electron microscopy(SEM),and energy dispersive X-ray spectroscopy(EDS)are used to characterize the physic-ochemical properties.The results show that the as-synthesizedβ-KSbF_(4)exhibits higher carrier concentra-tion of 1.0×10^(-6)S cm-Hz^(-1)K and hopping frequency of 1.31×10^(6)Hz at 30°C due to the formation of the fluorine vacancies.Meanwhile,the hopping frequency shows the same trend as the changes of ionic conductivity with the changes of temperature,while the carrier concentration is found to be almost con-stant.The two different trends indicate the hopping frequency is mainly responsible for the ionic conduc-tion behavior withinβ-KSbF_(4).Furthermore,the all-solid-state FIBs,in which Ag and Pb+PbF_(2)are adopted as cathode and anode,andβ-KSbF_(4)as fluoride ion conductor,are capable of reversible charge and discharge.The assembled FIBs show a discharge capacity of 108.4 mA h g^(-1)at 1st cycle and 74.2 mA h g^(-1)at 50th cycle.Based on an examination of the capacity decay mechanism,it has been found that deterioration of the electrolyte/electrode interface is an important reason for hindering the commer-c

关键词： Solid-state electrolyte Carrier concentration Hopping frequency β-KSbF_(4) All-solid-state fluoride ion batteries

Synergistic coupling among Mg_(2)B_(2)O_(5),polycarbonate and N,Ndimethylformamide enhances the electrochemical performance of PVDF-HFP-based solid electrolyte

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Journal of energy Chemistry 2024年第7期94卷 158-168页

作者： Yutong Jing Qiang Lv Yujia Chen Bo Wang Bochen Wu Cheng Li Shengbo Yang Zhipeng He Dianlong Wang Huakun Liu Shixue Dou miit key laboratory of Critical materials technology for new energy conversion and storage State Key Laboratory of Urban Water Resource and EnvironmentSchool of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001HeilongjiangChina Institute of energy Material Science University of Shanghai for Science and TechnologyShanghai 200093China Institute for Superconducting&Electronic materials Australian Institute of Innovative MaterialsUniversity of WollongongWollongongNSW 2500Australia

Polymer solid electrolytes(SPEs)based on the[solvate-Lit]complex structure have promising prospects in lithium metal batteries(LMBs)due to their unique ion transport mechanism.However,the solvation structure may compromise the mechanical performance and safety,hindering practical application of SPEs.In this work,a composite solid electrolyte(CSE)is designed through the organic-inorganic syner-gistic interaction among N,N-dimethylformamide(DMF),polycarbonate(PC),and Mg2B2Os in poly(vinyli-dene fluoride-co-hexafluoropropylene)(PVDF-HFP).Flame-retardant Mg_(2)B_(2)O_(5)nanowires provide non-flammability to the prepared CSEs,and the addition of PC improves the dispersion of Mg_(2)B_(2)O_(5) nanowires.Simultaneously,the organic-inorganic synergistic action of PC plasticizer and Mg_(2)B_(2)O_(5) nanowires pro-motes the dissociation degree of LiTFSI and reduces the crystallinity of PVDF-HFP,enabling rapid Li ion transport.Additionally,Raman spectroscopy and DFT calculations confirm the coordination between Mg atoms in Mg_(2)B_(2)O_(5) and N atoms in DMF,which exhibits Lewis base-like behavior attacking adjacent C-F and C-H bonds in PVDF-HFP while inducing dehydrofluorination of PVDF-HFP.Based on the syner-gistic coupling of Mg_(2)B_(2)O_(5),PC,and DMF in the PVDF-HFP matrix,the prepared CSE exhibits superior ion conductivity(9.78×10^(-4) s cm^(-1)).The assembled Li symmetric cells cycle stably for 3900 h at a current density of 0.1 mA cm^(-2) without short circuit.The LFPlILi cells assembled with PDL-Mg_(2)B_(2)O_(5)/PC CSEs show excellent rate capability and cycling performance,with a capacity retention of 83.3%after 1000 cycles at O.5 C.This work provides a novel approach for the practical application of organic-inorganic Synergistic CSEs in LMBs.

关键词： Composite solid electrolytes Safe Li metal batteries Synergistic coupling effect Poly(vinylidene fluoride-co-hexafluoropro pylene)