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High-selectivity electroreduction of low-concentration CO2 with large concentration fluctuation

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Science China Chemistry 2025年

作者： Mengyu Qi Yanbin Ma Chao Zhang Bingwei Li Xueqing Yang Zhaolin Shi Simeng Liu Changhua An Jiqing Jiao Tongbu Lu MOE International Joint laboratory of Materials Microstructure Analysis and Testing CenterInstitute for New Energy Materials and Low Carbon TechnologiesSchool of Materials Science and EngineeringSchool of Chemistry and Chemical EngineeringTianjin University of Technology Key laboratory of Advanced energy Materials Chemistry (Ministry of Education) Nankai University

Electrochemical CO2reduction reaction（CO2RR） has been regarded as one of the most promising solutions to achieving “zero carbon emission”. In most of the CO2RR-related studies, high-purity CO2has been employed as the feed gas; however, in practice, CO2is generally emitted in low concentrations, so it is of great significance to realize high-selectivity electroreduction of low-concentration CO2with large concentration fluctuation. In this work, we constructed a dual-active-site catalyst and successfully achieved CO2local enrichment and conversion for low-concentration CO2. Operando experiments reveal that the catalyst has one type of site for activating CO2and one type of site for binding the reaction intermediates. The dual-active-site catalyst displays a selectivity for formic acid consistently above 97% over a broad potential window（from-0.9 to-1.6 V ***）. Even when fed with a low-concentration CO2stream（volume ratio from 50% down to 10%）, the dual-active-site catalyst could display high activity and selectivity（>91%）. In particular, the selectivity is still above 85% when the CO2volume ratio is as low as 5%. This work offers a feasible route for converting low-concentration CO2via a synergistic effect for dual-active-site catalysts.

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Constructing Pr-doped CoOOH catalytic sites for efficient electrooxidation of 5-hydroxymethylfurfural

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Journal of energy Chemistry 2025年第1期100卷 234-244页

作者： Botao Fan Hao Zhang Bang Gu Feng Qiu Qiue Cao Wenhao Fang School of Chemical Science and Technology Yunnan University National Center for International Research on Photoelectric and energy Materials School of Materials and Energy Yunnan University

Electrocatalytic conversion of renewable biomass is emerging as a promising route for sustainable chemical production;hence it urgently calls for developing efficient electrocatalysts with low potentials and high current ***,a Pr-doped Co（OH）2hexagonal sheet （Pr/Co=1/9,in mole） is synthesized by electrodeposition as highly performant catalyst for 5-hydroxymethylfurfural （HMF） oxidation reaction（HMFOR） to produce 2,5-furandicarboxylic acid （FDCA）.This novel and low-cost catalyst possesses a rather low onset potential of 1.05 V （***） and requires only 1.10 V （***） to reach a current density of 10 mA cm-2for HMFOR,significantly outperforming Co（OH）2benchmark (i.e.,210 mV higher to reach10 m A cm-2).The origin of Pr promotion effect as well as the evolution of CoOOH catalytic sites and HMFOR process has been deeply elucidated by physical characterizations,kinetic experiments,in situ electrochemical techniques,and theoretical *** unique Pr-ameliorated CoOOH active centers enable 100%conversion of HMF,99.6%selectivity of FDCA,and 99.7%Faraday efficiency,with a superior cycling durability toward *** can be one of the most outstanding results for Co-based HMFOR catalysts to date in the *** this work can help open up new horizons for constructing novel and efficient Co-based electrocatalysts by the utilization of lanthanide elements.

关键词： Bioconversion

Asymmetric interfacial engineering regulated charge distribution on Ru/Ni-N-C sites for efficient hydrogen evolution reaction in alkaline and seawater electrolytes

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Science China Chemistry 2025年

作者： Rui Yu Xi Cao Chengyang Zhu Qingqing Chen Ziyi Yan Binbin Jiang Junjie Mao Xianwen Wei Key laboratory of Electrochemical Clean energy of Anhui Higher Education Institutes College of Chemistry and Materials ScienceAnhui Normal University Anhui Provincial Key laboratory of Advanced Catalysis and energy Materials School of Chemistry and Chemical Engineering Anqing Normal University School of Chemistry and Chemical Engineering Anhui University of Technology

Developing highly efficient and cost-effective electrocatalysts for hydrogen evolution reaction（HER） is grandly challenging in alkaline and alkaline seawater electrolytes. Herein, the asymmetric interfacial active sites with Ru nanoparticles and Ni single atoms in Ru/Ni-N-C were designed through a solvothermal-pyrolysis process. Constructing highly asymmetric interfacial active sites with a strong electron delocalization effect significantly improves HER kinetics. As expected, Ru/Ni-N-C requires low overpotentials with around 20 mV at 10 mA cm-2and robust durability over 48 h in alkaline and alkaline seawater *** at 200 mA cm-2, the overpotentials are close to 100 mV in both above electrolytes for Ru/Ni-N-C. Density function theory calculation results suggest that the asymmetric interface between Ru nanoparticle and Ni-N-C could accelerate the dissociation of water molecules and modulate the hydrogen species, consequently improving the HER performances. This work opens a unique approach for constructing advanced materials for energy conversion.

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Establishing a new testing protocol of the electrochemical stability window for electric double-layer capacitors

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Science China Chemistry 2025年第1期68卷 217-225页

作者： Ruilin Hou Xiaoxi Zhao Tingting Liang Qingyun Dou Shan Xu Xingbin Yan School of Materials Science and Engineering Sun Yat-sen University laboratory of Clean energy Chemistry and Materials Lanzhou Institute of Chemical Physics Chinese Academy of Sciences College of Engineering and Applied Sciences Nanjing University Center of Industrial Analysis and Testing Guangdong Academy of Science

The electrochemical stability window(ESW) is crucial for determining the energy density of electric double-layer capacitors(EDLCs). However, current ESW testing protocols of EDLCs are strongly affected by artificial factors, thereby leading to unreliable result. To solve this problem, we first identify the key shortcomings of the traditional protocols by analyzing their test principles. Subsequently, taking an aqueous carbon-based EDLC as an example, we design a side reaction descriptor to represent the response difference in the charging capacitance to side reactions between the cyclic voltammetry and galvanostatic chargedischarge methods. With the aid of this descriptor, we propose a new ESW testing protocol, which is not only able to completely avoid the adverse influence of subjective factors but also fully consider the operating condition limitations. The protocol can be extended from the single electrode to the full device. This work proposes a more rigorous definition of ESW and provides a reliable protocol for evaluating the ESW of EDLCs.

关键词： electric double-layer capacitors electrochemical stability window testing protocol side reaction descriptor operating limitation

Efficient and Stable Perovskite Solar Cells and Modules Enabled by Tailoring Additive Distribution According to the Film Growth Dynamics

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Nano-Micro Letters 2025年第2期17卷 387-400页

作者： Mengen Ma Cuiling Zhang Yujiao Ma Weile Li Yao Wang Shaohang Wu Chong Liu Yaohua Mai Institute of New energy Technology College of Physics&Optoelectronic EngineeringJinan UniversityGuangzhou 510632People’s Republic of China Key laboratory of New Semiconductors and Devices of Guangdong Higher Education Institutes Jinan UniversityGuangzhou 510632People’s Republic of China Guangdong Mellow energy Co. LimitedYuanming RoadZhuhai 519075GuangdongPeople’s Republic of China

Gas quenching and vacuum quenching process are widely applied to accelerate solvent volatilization to induce nucleation of perovskites in blade-coating *** this work,we found these two pre-crystallization processes lead to different order of crystallization dynamics within the perovskite thin film,resulting in the differences of additive *** then tailor-designed an additive molecule named 1,3-bis(4-methoxyphenyl)thiourea to obtain films with fewer defects and holes at the buried interface,and prepared perovskite solar cells with a certified efficiency of 23.75%.Furthermore,this work also demonstrates an efficiency of 20.18%for the large-area perovskite solar module(PSM)with an aperture area of 60.84 cm^(2).The PSM possesses remarkable continuous operation stability for maximum power point tracking of T_(90)>1000 h in ambient air.

关键词： Gas quenching Additive distribution Buried passivation Blade coating Crystallization dynamics

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Design of multifunctional interfaces on ceramic solid electrolytes for high-performance lithium-air batteries

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Green energy & Environment 2025年第1期10卷 183-192页

作者： Yunxin Shi Ziyang Guo Changhong Wang Mingze Gao Xiaoting Lin Hui Duan Yonggang Wang Xueliang Sun College of energy Material and Chemistry College of Chemistry and Chemical EngineeringInner Mongolia UniversityHohhot010021China Department of Mechanical and Materials Engineering Western UniversityLondonONN6A 5B9Canada Department of Chemistry and Shanghai Key laboratory of Molecular Catalysis and Innovative Materials Institute of New EnergyiChEM(Collaborative Innovation Center of Chemistry for Energy Materials)Fudan UniversityShanghai200433China Eastern Institute for Advanced Study Eastern Institute of TechnologyNingboZhejiang315100China

High-energy-density lithium(Li)–air cells have been considered a promising energy-storage system,but the liquid electrolyte-related safety and side-reaction problems seriously hinder their *** address these above issues,solid-state Li–air batteries have been widely ***,many commonly-used solid electrolytes generally face huge interface impedance inLi–air cells and also showpoor stability towards ambient air/Li ***,we fabricate a differentiating surface-regulated ceramic-based composite electrolyte(DSCCE)by constructing disparately LiI-containing polymethyl methacrylate(PMMA)coating and Poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP)layer on both sides of Li_(1.5)Al_(0.5)Ge_(1.5)(PO_(4))_(3)(LAGP).The cathode-friendly LiI/PMMA layer displays excellent stability towards superoxide intermediates and also greatly reduces the decomposition voltage of discharge products in Li–air ***,the anode-friendly PVDF-HFP coating shows low-resistance properties towards ***,Li dendrite/passivation derived from liquid electrolyte-induced side reactions and air/I-attacking can be obviously suppressed by the uniformand compact composite *** a result,the DSCCE-based Li–air batteries possess high capacity/low voltage polarization(11,836mAh g^(-1)/1.45Vunder 500mAg^(-1)),good rate performance(capacity ratio under 1000mAg^(-1)/250mAg^(-1) is 68.2%)and longterm stable cell operation(~300 cycles at 750 mA g^(-1) with 750 mAh g^(-1))in ambient air.

关键词： Li-air batteries Li_(1.5)Al_(0.5)Ge_(1.5)(PO_(4))_(3) Polymers Composite electrolyte Ambient air

Low‑Temperature Fabrication of Stable Black‑Phase CsPbI_(3)Perovskite Flexible Photodetectors Toward Wearable Health Monitoring

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Nano-Micro Letters 2025年第3期17卷 232-245页

作者： Yingjie Zhao Yicheng Sun Chaoxin Pei Xing Yin Xinyi Li Yi Hao Mengru Zhang Meng Yuan Jinglin Zhou Yu Chen Yanlin Song College of Chemistry and Pingyuan laboratory Zhengzhou UniversityZhengzhou 450001People’s Republic of China Key laboratory of Green Printing Institute of ChemistryChinese Academy of SciencesBeijing 100190People’s Republic of China Key laboratory of Bio‑Inspired Materials and Interfacial Science Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190People’s Republic of China Institute of High energy Physics Chinese Academy of SciencesBeijing 100049People’s Republic of China

Flexible wearable optoelectronic devices fabricated fromorganic–inorganic hybrid perovskites significantly accelerate the developmentof portable energy,biomedicine,and sensing fields,but their poor thermal stabilityhinders further ***,all-inorganic perovskites possessexcellent thermal stability,but black-phase all-inorganic perovskite filmusually requires high-temperature annealing steps,which increases energy consumptionand is not conducive to the fabrication of flexible wearable *** this work,an unprecedented low-temperature fabrication of stable blackphaseCsPbI3perovskite films is demonstrated by the in situ hydrolysis reactionof diphenylphosphinic chloride *** released diphenyl phosphateand chloride ions during the hydrolysis reaction significantly lower the phasetransition temperature and effectively passivate the defects in the perovskitefilms,yielding high-performance photodetectors with a responsivity of 42.1 AW−1 and a detectivity of 1.3×10^(14)***,high-fidelity imageand photoplethysmography sensors are demonstrated based on the fabricated flexible wearable *** work provides a newperspective for the low-temperature fabrication of large-area all-inorganic perovskite flexible optoelectronic devices.

关键词： In situ hydrolyzation Low-temperature processing All-inorganic perovskite Flexible photodetectors Health monitoring

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Automatic and Rapid Throughflow-Based Optimal Design Method for Multi-Stage Axial-Flow Compressors

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Journal of Thermal Science 2025年第1期34卷 77-91页

作者： LEI Fan ZHANG Xiawen JU Yaping ZHANG Chuhua Department of Fluid Machinery and Engineering School of Energy and Power EngineeringXi'an Jiaotong University Production and Environmental Department China Huaneng Group.Co.Ltd. State Key laboratory for Strength and Vibration of Mechanical Structures Xi'an Jiaotong University

Throughflow design has the advantages of less time consumption and large optimization space,and thus is the corner stone of advanced design system of multi-stage axial-flow *** majority of relevant studies were limited to the throughflow inverse designs,and quite few works have been till now devoted to the throughflow optimal *** this work,an automatic and rapid throughflow-based optimal design method is proposed for axial-flow compressors in which a throughflow inverse design solver is embedded in optimal genetic algorithm to improve the design efficiency of axial-flow *** types of design parameters in the throughflow inverse design of axial-flow compressors,i.e.,swirl and shroud curve,are simultaneously used to optimize both the blade shape and flow *** proposed method is validated by the redesign optimization of the benchmark axial-flow compressor NASA Stage 35,and the CFD predictions show that the throughflow-based optimization leads to 1.18% efficiency benefit at design *** proposed method is then utilized to the two-dimensional throughflow optimal design of a large-scale 6.5-stage axial-flow industrial *** optimal design results are confirmed by CFD predictions,indicating that the proposed method can effectively improve the design adiabatic efficiency of the compressors by 1.09% within a few minutes on desk-top *** throughflow design implications are also obtained for advanced axial-flow industrial *** work could enhance the capability of throughflow design method and has engineering application value to explore the throughflow optimization space of multi-stage axial-flow compressors.

关键词： NASA

CoTCPP integrates with BiOBr microspheres for improved solar-driven CO_(2)reduction performance

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Green energy & Environment 2025年第1期10卷 193-202页

作者： Lina Li Yi Zhang Gaopeng Liu Tiange Wei Junze Zhao Bin Wang Mengxia Ji Yuanbin She Jiexiang Xia Huaming Li School of Chemistry and Chemical Engineering Institute for Energy ResearchJiangsu University301 Xuefu RoadZhenjiang212013China State Key laboratory Breeding Base of Green Chemistry-Synthesis Technology College of Chemical EngineeringZhejiang University of TechnologyHangzhou310014China

CO_(2) photoreduction into carbon-based chemicals has been considered as an appropriate way to alleviate the energy issue and greenhouse ***,the 5,10,15,20-tetra(4-carboxyphenyl)porphyrin cobalt(II)(CoTCPP)has been integrated with BiOBr microspheres and formed the CoTCPP/BiOBr *** as-prepared CoTCPP/BiOBr-2 composite shows optimized photocatalytic performance for CO_(2) conversion into CO and CH_(4) upon irradiation with 300 W Xe lamp,which is 2.03 and 2.58 times compared to that of BiOBr,*** introduced CoTCPP significantly enhanced light absorption properties,promoted rapid separation of photogenerated carriers and boosted the chemisorption of CO_(2) *** metal Co^(2+) at the center of the porphyrin molecules also acts as adsorption center for CO_(2) molecules,accelerating the CO_(2) conversion into CO and *** possible mechanism of CO_(2) photoreduction was explored by in-situ FT-IR *** work offers a new possibility for the preparation of advanced photocatalysts.

关键词： BiOBr CoTCPP CO_(2)photoreduction Carriers transfer CO_(2)adsorption-activation