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Atmospheric chemistry of 2-nitrobenzaldehyde:Initiated by photo-excitation,OH-oxidation,and small TiO_(2) clusters adsorption catalysis

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Journal of Environmental Sciences 2024年第5期139卷 123-137页

作者： Feng-Yang Bai Xiang-Huan Liu Ting-Ting Meng Zhou Yu Yi-Chen Wang Shuang Ni Zhen Zhao institute of Catalysis for energy and Environment College of Chemistry and Chemical EngineeringShenyang Normal UniversityShenyang 110034China

The fate of 2-nitrobenzaldehyde(2-NBA)is of interest in atmospheric chemistry as it is a semi-volatile organic compound with high photosensitivity.This study presents a quantum chemical study of the gas-phase reactions of 2-NBA photo-excitation and OH-oxidation in the absence and presence of small TiO_(2) clusters.To further understand the unknown photolysis mechanism,the photo-reaction pathways of ground singlet state and the lying excited triplet state of 2-NBA were investigated including the initial and subsequent reactions of proton transfer,direct CO,NO_(2),and HCO elimination routes in the presence of O_(2) and NO.Meanwhile,the OH-mediated degradation of 2-NBA proceeded via five H-extraction and six OH-addition channels by indirect mechanism,which follows a succession of reaction steps initiated by the formation of weakly stable intermediate complexes.The H-extraction from the-CHO group was the dominant pathway with a negative activation energy of-1.22 kcal/mol.The calculated rate coefficients at 200–600 K were close to the experimental data in literature within 308-352 K,and the kinetic negative temperature independence was found in both experimental literature and computational results.Interestingly,2-NBA was favored to be captured onto small TiO_(2) clusters via six adsorption configurations formed via various combination of three types of bonds of Ti…O,Ti…C,and O…H between the molecularly adsorbed 2-NBA and TiO_(2) clusters.Comparison indicted that the chemisorptions of aldehyde oxygen have largest energies.The results suggested adsorption conformations have a respectable impact on the catalysis barrier.This study is significant for understanding the atmospheric chemistry of 2-nitrobenzaldehyde.

关键词： 2-nitrobenzaldehyde OH radical oxidation Rate coefficient Photolysis mechanism Adsorption catalysis

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Printable oil-NiO_(X)hole transport layer enables efficient n-i-p perovskite solar cells with a high thermal stability

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Science China chemistry 2024年第7期67卷 2335-2340页

作者： Yazhou Xu Zhaoyang Chu Hongyu Wang Zhi Xing Baojin Fan Xiaotian Hu Yiwang Chen College of chemistry and Chemical Engineering/institute of Polymers and energy chemistry(IPEC)/Film energy chemistry for Jiangxi Provincial Key Laboratory(FEC) Nanchang UniversityNanchang 330031China Key Lab of Fluorine and Silicon for energy Materials and chemistry of Ministry of Education Jiangxi Normal University Nanchang 330022China Peking University Yangtze Delta institute of Optoelectronics Nantong 226010China

Currently,highly efficient n-i-p perovskite solar cells rely on an organic interface layer for high efficiency,especially 2,2',7,7'-tetrakis[N,N-bis(4-methoxyphenyl)ami-no]-9,9′-spirobifluorene(spiro-OMeTAD),but the instability of organic materials in the photothermal field compromises device stability.In this study,we employ the oleic acid(YS)/oleamine(YA)end-sealing method to achieve uniform dispersion of NiO_(X)nanoparticles,effectively mitigating coagulation resulting from high local concentration and secondary motion adsorption.Furthermore,the conductivity of the hole transport layer and its energy level alignment with perovskite is enhanced by the additional 2,3,5,6-tetrafluoro-7,7',8,8'-tetracyanodimethyl-p-benzoquinone(F4TCNQ),leading to a remarkable improvement of open-circuit voltage and fill factor,thus the high efficiency of 25.17%and 24.36%on 0.1 and 1.01cm2,respectively.Moreover,by realizing an all-inorganic interface layer,an initial efficiency exceeding 90%is maintained even after 2,800 h of heating at 85℃.

关键词： oil-NiO_(X) perovskite solar cells printing technology high efficiency thermal stability

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Utilizing a metal-forging inspired chain combing strategy to enhance properties and expand applications of Nylon 66 plastic via heat inducing

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Nano Research 2024年第3期17卷 2164-2171页

作者： Junyu Yang Jiangwei Zhang Nan Wang Guangyuan Zhou Division of energy Materials Daglian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Innovation Center of energy Material and chemistry College of Chemistry and Chemical EngineeringInner Mongolia UniversityHohhot 010021China

The mechanical properties of engineering plastics can be enhanced through effective surface mechanical treatment(SMT),which can be applied to various types of engineering plastics,eliminating the limitations of conventional polymer processing and could potentially extend their applications and improve their performance and reliability as structural-functional materials.Inspired by metal forging,this work proposes a simple and effective SMT strategy to enhance the mechanical properties of polyamide 66(PA66).Tensile tests have shown that SMTed PA66 samples exhibit significant improvements in both Young’s modulus and ultimate tensile strength(UTS),with a 2104 MPa Young’s modulus,almost double that of the pristine samples,and a 35.56%increase in UTS,reaching 183 MPa.Additionally,the modulus within the localized SMTed surface layer could reach up to 14 GPa,which is approximately 14 times higher than that of the pristine sample.The Vickers hardness within the localized SMTed surface layer can be doubled,reaching 10.72 Hv,and the crystallinity can increase by approximately 20%compared to the untreated region.Furthermore,force field molecular dynamics(FFMD)simulations were conducted to investigate the ternary relationship between the SMT method,PA66’s molecular structure,and its properties.The combination of MD simulations and versatile structural characterizations provides evidence that the SMT method’s mechanism,under heat induction,results in a chain-combing procedure that changes the polymer’s molecular morphology microscopically and enhances its mechanical properties macroscopically.

关键词： Nylon 66 mechanical properties hardness crystallinity structural characterizations molecular dynamics simulation

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Ti_(3)C_(2)T_(x)MXene wrapped,carbon-coated porous Si sheets for improved lithium storage performance

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Chinese Chemical Letters 2024年第2期35卷 617-621页

作者： Hui Cheng Yueming Liu Zhongling Cheng Xianying Wang Na Huang Haijiao Zhang institute of Nanochemistry and Nanobiology School of Environmental and Chemical EngineeringShanghai UniversityShanghai 200444China Shanghai Key Laboratory of Green chemistry and Chemical processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062China energy Materials Research Center AG Hydrogen Materials & Devices CAS Key Laboratory of Materials for Energy ConversionShanghai Institute of CeramicsChinese Academy of Sciences (SICCAS)Shanghai 200050China

Si-based materials have shown great potential as lithium-ion batteries(LIBs)anodes due to their natural reserves and high theoretical capacity.However,the large volume changes during cycles and poor conductivity of Si lead to rapid capacity decay and poor cycling stability,ultimately limiting their commercial applications.Herein,we have skillfully utilized the microporous MCM-22 zeolite as the unique silicon source to produce porous Si(pSi)sheets by a simple magnesiothermic reduction,followed by a carbon coating and further Ti_(3)C_(2)T_(x)MXene assembly,obtaining the ternary pSi@NC@TNSs composite.In the design,porous Si sheets provide more active sites and shorten Li-ion transport paths for electrochemical reactions.The N-doped carbon(NC)layer serves as a bonding layer to couple pSi and Ti_(3)C_(2)T_(x).The conductive network formed by 2D Ti_(3)C_(2)T_(x)and medium NC layer effectively enhances the overall charge transport of the electrode material,and helps to stabilize the electrode structure.Therefore,the as-made pSi@NC@TNSs anode delivers an improved lithium storage performance,exhibiting a high reversible capacity of 925 mAh/g at 0.5 A/g after 100 cycles.This present strategy provides an effective way towards high-performance Si-based anodes for LIBs.

关键词： Si anodes Ti_(3)C_(2)Ti_(x)MXene Porous structure Interfacial assembly Lithium-ion batteries

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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

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Multifunctional photon conversion materials for enhancing silicon solar cells

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Light(Science & Applications) 2024年第4期13卷 598-601页

作者： Yiyan Zhang Guanying Chen MIIT Key Laboratory of Critical Materials Technology for New energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of Technology150001 HarbinChina

A type of multifunctional erbium(Er^(3+))and ytterbium(Yb^(3+))codoped NaY(WO4)2 phosphors,with simultaneous photon upconversion,photon quantum cutting,and luminescence ratiometric temperature sensing abilities,have b... 详细信息

关键词： photon luminescence quantum

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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

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Classification and technical target of water electrolysis for hydrogen production

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Journal of energy chemistry 2024年第8期95卷 554-576页

作者： Kahyun Ham Sooan Bae Jaeyoung Lee Ertl Center for Electrochemistry and Catalysis Gwangju Institute of Science and Technology(GIST) Department of Heterogeneous Reactions Max Planck Institute for Chemical Energy Conversion School of Earth Sciences and Environmental Engineering GIST International Future Research Center of Chemical energy Storage and Conversion processes GIST eSuS Co. Ltd. #408 S6 Building School of Environment and Energy Engineering GIST

Continuous efforts are underway to reduce carbon emissions worldwide in response to global climate change. Water electrolysis technology, in conjunction with renewable energy, is considered the most feasible hydrogen production technology based on the viable possibility of large-scale hydrogen production and the zero-carbon-emission nature of the process. However, for hydrogen produced via water electrolysis systems to be utilized in various fields in practice, the unit cost of hydrogen production must be reduced to $1/kg H2. To achieve this unit cost, technical targets for water electrolysis have been suggested regarding components in the system. In this paper, the types of water electrolysis systems and the limitations of water electrolysis system components are explained. We suggest guideline with recent trend for achieving this technical target and insights for the potential utilization of water electrolysis technology.

关键词： Electrochemistry Hydrogen production Technical target Water electrolysis

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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

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Delving into the dissimilarities in electrochemical performance and underlying mechanisms for sodium and potassium ion storage in N-doped carbon-encapsulated metallic Cu2Se nanocubes

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Journal of energy chemistry 2024年第8期95卷 336-347页

作者： Xinyu Wang Yanan Xu Xiaofeng Liu Lei Tan Huaiqiang Gu Xin Du Dan Li College of chemistry Zhengzhou University Green Catalysis Center College of Chemistry Zhengzhou University institute of Theoretical Physics Lanzhou University School of Nuclear Science and Technology Lanzhou University Key Laboratory of Advanced energy Materials chemistry(Ministry of Education) College of Chemistry Nankai University State Key Laboratory of chemistry and Utilization of Carbon Based energy Resources College of Chemistry Xinjiang University

The large volumetric variations experienced by metal selenides within conversion reaction result in inferior rate capability and cycling stability,ultimately hindering the achievement of superior electrochemical performance.Herein,metallic Cu2Se encapsulated with N-doped carbon（Cu2Se@NC） was prepared using Cu2O nanocubes as templates through a combination of dopamine polymerization and hightemperature selenization.The unique nanocubic structure and uniform N-doped carbon coating could shorten the ion transport distance,accelerate electron/charge diffusion,and suppress volume variation,ultimately ensuring Cu2Se@NC with excellent electrochemical performance in sodium ion batteries（SIBs） and potassium ion batteries（PIBs）.The composite exhibited excellent rate performance(187.7 mA h g-1at 50 A g-1in SIBs and 179.4 mA h g-1at 5 A g-1in PIBs) and cyclic stability(246,8 mA h g-1at 10 A g-1in SIBs over 2500 cycles).The reaction mechanism of intercalation combined with conversion in both SIBs and PIBs was disclosed by in situ X-ray diffraction（XRD） and ex situ transmission electron microscope（TEM）.In particular,the final products in PIBs of K2Se and K2Se3species were determined after discharging,which is different from that in SIBs with the final species of Na2Se.The density functional theory calculation showed that carbon induces strong coupling and charge interactions with Cu2Se,leading to the introduction of built-in electric field on heterojunction to improve electron mobility.Significantly,the theoretical calculations discovered that the underlying cause for the relatively superior rate capability in SIBs to that in PIBs is the agile Na+diffusion with low energy barrier and moderate adsorption energy.These findings offer theoretical support for in-depth understanding of the performance differences of Cu-based materials in different ion storage systems.

关键词： Cu2Se nanocubes DFT calculations Ion storage mechanism Potassium ion batteries Sodium ion batteries

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