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A low-cost wide bandgap polymer based on carboxylate substituted thiazole enables efficient organic solar cells with remarkable batch-to-batch reproducibility

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Science China Chemistry 2025年第2期68卷 733-744页

作者： Xiaodong Zhu Yuchen Lei Jianhong Gao Yanjun He Jinsicheng Liu Qian Guo Xiang Gao Liwei Xiong Xunchang Wang Renqiang Yang Zhitian Liu Hubei Engineering Technology research center of Optoelectronic and New energy materials Hubei Key Laboratory of Plasma Chemistry and Advanced MaterialsSchool of Materials Science and EngineeringWuhan Institute of TechnologyWuhan 430205China Key Laboratory of Optoelectronic Chemical materials and Devices(Ministry of Education) School of Optoelectronic Materials&TechnologyJianghan UniversityWuhan 430056China

Constructing the low-cost,high-efficiency,and good batch-to-batch reproducibility polymer donor is vitally important for the application of organic solar ***,we develop a structurally simple carboxylate-substituted thiazole as an electronwithdrawing building block to construct a low-cost polymer,PBTTzE,containing a facilely prepared chlorinated benzo[1,2-b:4,5-b′]dithiophene(BDTCl)donor *** from synergistic electron deficient effects of chlorination and ester group and C=N,as well as the noncovalent interaction of S…O and S…N,PBTTzE exhibits a deep HOMO energy level(−5.59 eV),and a planar skeleton *** combined with the IT-4F acceptor,the polymer(54 kDa)demonstrated a champion PCE of 15.87%,which is the highest value in the IT-4F-based binary devices to ***,PBTTzE exhibits excellent batch-tobatch reproducibility due to its very similar PCEs within a range of 43–76 *** addition,an alloyed state and complementary absorption can be formed between PM6 and ***,in a ternary device with PBTTzE added to the PM6:BTP-eC9 blend,a top PCE of 18.76%is achieved due to the suppressed energy loss,prolonged exciton diffusion distance,and improved charge *** work demonstrates that the carboxylate-substituted thiazole is a highly promising acceptor unit for constructing low-cost and high-performance polymers.

关键词： carboxylate substituted thiazole polymer donor low-cost batch-to-batch reproducibility organic solar cells

Improving performance of perovskite solar cells enabled by defects passivation and carrier transport dynamics regulation via organic additive

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Chinese Chemical Letters 2025年第2期36卷 551-556页

作者： Rongjun Zhao Tai Wu Yong Hua Yude Wang Department of Physics Center for Optoelectronics Engineering ResearchYunnan University Yunnan Key Laboratory for Micro/Nano materials&Technology International Joint Research Center for Optoelectronic and Energy MaterialsSchool of Materials and EnergyYunnan University Yunnan Key Laboratory of Carbon Neutrality and Green Low-carbon Technologies Yunnan University

Defects at the grain boundaries(GBs) of perovskite film highly restrict both the efficiency and stability of perovskite solar cells(PSCs). Herein, organic small molecules of butanedioic acid(BA) and acetylenedicarboxylic acid(AA), containing two carbonyl(C=O) groups and different core-units, were incorporated into perovskite as additives for PSCs application. Thanks to the strong coordination interaction between C=O group and under-coordinated Pb2+, the additives can effectively passivate film defects and regulate the perovskite crystallization, yielding high-quality perovskite films with lower defect densities. More importantly, the additives can efficiently regulate the charge transport behaviors in PSCs. Benefiting from the defects passivation and the regulation of charge carrier dynamics, the BA and AA-treaded PSCs show the power conversion efficiencies of 21.52% and 20.50%, which are higher than that of the control device(19.41%). Besides, the optimal devices exhibit a remarkable enhanced long-term stability and moisture tolerance compared to the pristine devices. Furthermore, the transient absorption spectrum reveals the mechanism of enhanced photovoltaic performances, attributing to the improvement of charge transport capability at the perovskite/Spiro-OMeTAD interfaces. This work affords a promising strategy to improve the efficiency and stability of PSCs through regulating the charge-carrier dynamic process in perovskite film.

关键词： Additives Carrier dynamics Defects passivation Perovskite solar cells Stability

Efficient photocatalytic H2 evolution over tubular mesoporous carbon nitride with N-vacancy by microwave-assisted synthesis

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Science China Chemistry 2025年第3期 866-873页

作者： Yuanlong Pan Qiang Zhang Guangzheng Huang Yannan Luo Honglin Gao School of materials and energy National Center for International Research on Photoelectric and Energy MaterialsYunnan University

Modifying the microstructure of photocatalysts while simultaneously introducing vacancies has shown significant potential in enhancing their performance for hydrogen ***,a novel tubular mesoporous carbon nitride（TMCN） with nitrogen vacancies was fabricated using a microwave-assisted synthesis strategy,employing melamine-cyanuric acid supramolecular（MC-S） as the *** optimized TMCN exhibited an outstanding H2production rate,approximately 29 times higher than that of pristine *** N-vacancies serve as sites for reactant adsorption and activation,leading to enhanced delocalization of ***,the porous structures of TMCN facilitate the reactant diffusion,while its tubular architectures promote the oriented transfer of charge ***,the markedly improved photocatalytic performance of TMCN can be predominantly attributed to the synergistic effects arising from its superior structure and N-vacancy *** work opens new possibilities for the simultaneous formation of surface defect states as photocatalytic reaction sites and distinctive structures conducive to charge carrier transport.

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Biomimetic proton pocket and effective interfacial modulation for zinc metal anodes

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Science China Chemistry 2025年第2期68卷 526-535页

作者： Qi Dong Qingshun Nian Xuan Luo Jiajia Fan Jinyu Jiang Zhuangzhuang Cui Digen Ruan Xiaodi Ren Hefei National research center for Physical Sciences at the Microscale CAS Key Laboratory of Materials for Energy ConversionDepartment of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China

Rechargeable aqueous zinc batteries(RAZBs)offer a promising solution for large-scale energy storage due to the abundance,low cost,and safety of ***,practical applications are hindered by Zn anode instability,dendrite growth,and hydrogen evolution reactions(HER).Chaotropic Zn(ClO_(4))2 electrolytes are favorable for low-temperature operations but exacerbate these issues due to their high acidity,leading to severe Zn corrosion and layered double hydroxide *** propose a biomimetic strategy using methylguanidoacetic acid(creatine)as a low-cost,eco-friendly additive to address these *** acts as a proton pocket to finely tune the pH of acidic Zn(ClO_(4))2 electrolytes for suppressing HER and stabilizing the Zn ***,the formed creatinine cations adsorb on the Zn surface,promoting highly controlled Zn deposition with a preferred(002)*** approach significantly enhances battery cycling performance,with Zn||Zn cells demonstrating extended cycling stability at both low and high current ***||Cu cells exhibited improved Coulombic efficiency over thousands of cycles,indicating highly reversible Zn plating/***,stable cell operations were realized at the temperature as low as−35℃ without electrolyte *** findings highlight the potential of biomimetic proton regulation and interfacial modulation for improving the stability and reversibility of Zn plating/stripping in RAZBs.

关键词： zinc metal anode dendrite suppression interfacial modulation proton-triggered cyclization Zn(ClO_(4))2 electrolyte

Structure-phase transformation of bismuth oxide to Ta-Bi_(24)O_(31)Cl_(10)shoulder-by-shoulder heterojunctions for efficient photocatalytic removal of antibiotic

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Journal of Environmental Sciences 2025年第3期149卷 149-163页

作者： Man Yang Zhenzhen Shi Shaodong Sun Bian Yang Jie Cui Jianing Li Daqin Yun Nian Lei Engineering research center of Conducting materials and Composite Technology Ministry of EducationShaanxi Engineering Research Center of Metal-Based Heterogeneous Materials and Advanced Manufacturing TechnologyShaanxi Province Key Laboratory for Electrical Materials and Infiltration TechnologySchool of Materials Science and EngineeringXi’an University of TechnologyXi’an 710048China College of energy Xiamen UniversityXiamen 361005China Beijing Key Laboratory of Ionic Liquids Clean Process Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China

Developing heterojunction photocatalyst with well-matched interfaces andmultiple charge transfer paths is vital to boost carrier separation efficiency for photocatalytic antibiotics removal,but still remains a great *** present work,a new strategy of chloride anion intercalation in Bi_(2)O_(3)via one-pot hydrothermal process is *** as-prepared Ta-BiOCl/Bi_(24)O_(31)Cl_(10)(TBB)heterojunctions are featured with Ta-Bi_(24)O_(31)Cl_(10)and Ta-BiOCl lined shoulder-by-shouleder via semi-coherent *** this TBB heterojunctions,the well-matched semi-coherent interfaces and shoulder-by-shoulder structures provide fast electron transfer andmultiple transfer paths,respectively,leading to enhanced visible light response and improved photogenerated charge ***,a type-II heterojunction for photocharge separation has been obtained,in which photogenerated electrons are drove from the CB(conduction band)of Ta-Bi_(24)O_(31)Cl_(10)to the both of bilateral empty CB of Ta-BiOCl and gathered on the CB of Ta-BiOCl,while the photogenerated holes are left on the VB(valence band)of Ta-Bi_(24)O_(31)Cl_(10),effectively hindering the recombination of photogenerated electron-hole ***,the separated electrons can effectively activate dissolved oxygen for the generation of reactive oxygen species(·O_(2)^(−)).Such TBB heterojunctions exhibit remarkably superior photocatalytic degradation activity for tetracycline hydrochloride(TCH)solution to Bi_(2)O_(3),Ta-BiOCl and Ta-Bi_(24)O_(31)Cl_(10).This work not only proposes a Ta-BiOCl/Bi_(24)O_(31)Cl_(10)shoulder-by-shoulder micro-ribbon architectures with semi-coherent interfaces and successive type-Ⅱheterojunction for highly efficient photocatalytic activity,but offers a new insight into the design of highly efficient heterojunction through phasestructure synergistic transformation strategy.

关键词： Heterojunction Bismuth oxide Charge separation/transfer Photocatalytic degradation Catalytic mechanism

Improving the reliability of classical molecular dynamics simulations in battery electrolyte design

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Journal of energy Chemistry 2025年第2期101卷 34-41页

作者： Xin He Yujie Zhang Haomiao Li Min Zhou Wei Wang Ruxing Wang Kai Jiang Kangli Wang State Key Laboratory of advanced Electromagnetic Technology School of Electrical and Electronic Engineering Huazhong University of Science and Technology State Key Laboratory of materials Processing and Die & Mould Technology College of Materials Science and Engineering Huazhong University of Science and Technology Hubei Collaborative Innovation center for High-efficiency Utilization of Solar energy Hubei University of Technology

Explorations into new electrolytes have highlighted the critical impact of solvation structure on battery performance,Classical molecular dynamics(CMD) using semi-empirical force fields has become an essential tool for simulating solvation ***,mainstream force fields often lack accuracy in describing strong ion-solvent interactions,causing disparities between CMD simulations and experimental *** some empirical methods have been employed in some of the studies to address this issue,their effectiveness has been *** CMD research,supported by quantum chemical calculations and experimental data,reveals that the solvation structure is influenced not only by the charge model but also by the polarization *** empirical approaches that focused solely on adjusting ion-solvent interaction strengths overlooked the importance of polarization *** on this insight,we propose integrating the Drude polarization model into mainstream force fields and verify its feasibility in carbonate,ether,and nitrile *** experimental results demonstrate that this approach significantly enhances the accuracy of CMD-simulated solvation *** work is expected to provide a more reliable CMD method for electrolyte design,shielding researchers from the pitfalls of erroneous simulation outcomes.

关键词： Classical molecular dynamics Electrolyte Simulations Solvation structure

Platinum modification of metallic cobalt defect sites for efficient electrocatalytic oxidation of 5-hydroxymethylfurfural

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Journal of energy Chemistry 2025年第2期101卷 463-473页

作者： Haoyu Zhan Baixue Cheng Yankun Lu Danning Xing Xingshuai Lv Huining Huang Thomas Frauenheim Tao Wang Peng Zhou State Key Laboratory of Bio-fibers and Eco-textiles College of Materials Science and Engineering Collaborative Innovation Center of Shandong Marine Biobased Fibers and Ecological Textiles Institute of Marine Biobased Materials Qingdao University Shandong Institute of advanced Technology College of Chemistry and Chemical Engineering Ocean University of China Tianjin Key Laboratory of advanced Functional Porous materials Institute for New Energy Materials & Low-Carbon Technologies School of Materials Science and EngineeringTianjin University of Technology School of Science Constructor University Beijing Computational Science research center College of Chemistry and Molecular Engineering Qingdao University of Science and Technology

Co3O4possesses both direct and indirect oxidation effects and is considered as a promising catalyst for the oxidation of 5-hydroxymethylfurfural（HMF）.However,the enrichment and activation effects of Co3O4on OH-and HMF are weak,which limits its further *** defect engineering can regulate the electronic structure,optimize the adsorption of intermediates,and improve the catalytic activity by breaking the symmetry of the material,which is rarely involved in the upgrading of *** this work,we prepare Co3O4with metal defects and load the precious metal platinum at the defect sites（PtVco）.The results of in-situ characterizatio ns,electrochemical measurements,and theoretical calculations indicate that the reduction of Co-Co coordination number and the formation of Pt-Co bond induce the decrease of electron filling in the antibonding orbitals of Co *** resulting upward shift of the d-band center of Co combined with the characteristic adsorption of Pt species synergically enhances the enrichment and activation of organic molecules and OH species,thus exhibiting excellent HMF oxidation activity(including a lower onset potential（1.14 V） and 19 times higher current density than pure Co3O4at 1.35 V).In summary,this work explores the adsorption enhancement mechanism of metal defect sites modified by precious metal in detail,provides a new option for improving the HMF oxidation activity of cobalt-based materials,broadens the application field of metal defect based materials,and gives an innovative guidance for the functional utilization of metal defect sites in biomass conversion.

关键词： Adsorption enhancement Biomass upgrading Coordination environment Electrocatalysis Metallic defect

Constructing electrochemically stable single crystal Ni-rich cathode material via modification with high valence metal oxides

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Journal of energy Chemistry 2025年第02期101卷 392-401页

作者： Hancheng Shi Jiongzhi Zheng Tao Wan Hongqiang Wang Zeping Wen Fenghua Zheng Mingru Su Aichun Dou Yu Zhou Ahmad Naveed Panpan Zhang Hailong Wang Ruiqiang Guo Yunjian Liu Dewei Chu School of Material Science and Engineering Jiangsu University Thayer School of Engineering Dartmouth College School of materials Science and Engineering The University of New South Wales School of Chemistry and Pharmaceutical Sciences Guangxi Normal University School of materials and New energy Ningxia University Thermal Science research center Shandong Institute of Advanced Technology

Single crystal Ni-rich cathode materials（SCNCM） are a good supplement in the market of nickel-based materials due to their safety and excellent electrochemical ***,the challenges of cation mixing,phase change during charge/discharge,and low thermal stability remain unresolved in single crystal *** address these issues,SCNCM are rationally modified by incorporating transition metal（TM） oxides,and the influence of metal ions with different valence states on the electrochemical properties of SCNCM is methodically explored through experimental results and theoretical *** structural stability is demonstrated in SCNCM after the modifications,and the degree of improvement in the matrix materials varies depending on the valence state of doped TM *** highest structural stability is found in WO3-modified SCNCM,due to the smaller effective ion radii,higher electro-negativity,stronger W-O bond,and efficient suppression of oxygen vacancy *** a result,WO3-modified SCNCM have outstanding cycle performance,with a capacity retention rate of90.2% after 200 *** study provides an insight into the design of advanced SCNCM with enhanced reversibility and cyclability.

关键词： In-situ coating Ion doping Lithium-ion battery Single crystal Ni-rich material Strengthening mechanism analysis

Building Li-S batteries with enhanced temperature adaptability via a redox-active COF-based barrier-trapping electrocatalyst

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Journal of energy Chemistry 2025年第2期101卷 702-712页

作者： Jie Xu Acheng Zhu Zhangyu Zheng Yiming Qi Yuwen Cheng Yongjie Cao Bo Peng Lianbo Ma Yonggang Wang School of materials Science and Engineering Key Laboratory of Efficient Conversion and Solid-state Storage of Hydrogen & Electricity of Anhui Province Key Laboratory of Green Fabrication and Surface Technology of Advanced Metal Materials of Ministry of Education Anhui University of Technology Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative materials Institute of New Energy iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Fudan University

Covalent organic frameworks（COFs） are promising materials for mitigating polysulfide shuttling in lithium-sulfur（Li-S） batteries,but enhancing their ability to convert polysulfides across a wide temperature range remains a challenge,Herein,we introduce a redox-active COF（RaCOF） that functions as both a physical barrier and a kinetic enhancer to improve the temperature adaptability of Li-S batteries,The RaCOF constructed from redox-active anthraquinone units accelerates polysulfide conversion kinetics through reversible C=O/C-OLi transformations within a voltage range of 1,7 to 2.8 V（***+/Li）,optimizing sulfur redox reactions in ether-based *** conventional COFs,RaCOF provides bidentate trapping of polysulfides,increasing binding energy and facilitating more effective polysulfide ***-situ XRD and ToF-SIMS analyses confirm that RaCOF enhances polysulfide adsorption and promotes the transformation of lithium sulfide（Li2S）,leading to better sulfur cathode ***,RaCOF-modified Li-S batteries demonstrate low self-discharge（4.0% decay over a 7-day rest）,excellent wide-temperature performance（stable from-10 to+60℃）,and high-rate cycling stability（94% capacity retention over 500 cycles at 5.0 C）.This work offers valuable insights for designing COF structures aimed at achieving temperature-adaptive performance in rechargeable batteries.

关键词： Covalent organic framework Lithium-sulfur batteries Redox-active property Wide-temperature adaptability