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Modulating d-d orbitals coupling in PtPdCu medium-entropy alloy aerogels to boost pH-general methanol electrooxidation performance

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Chinese chemical Letters 2025年第4期36卷 221-228页

作者： Kaili Wang Pengcheng Liu Mingzhe Wang Tianran Wei Jitao Lu Xingling Zhao Zaiyong Jiang Zhimin Yuan Xijun Liu Jia He School of Chemistry&Chemical Engineering and Environmental Engineering Weifang UniversityWeifang 261061China School of Chemistry and Chemical Engineering Tianjin University of TechnologyTianjin 300384China State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured MaterialsSchool of ResourcesEnvironment and MaterialsGuangxi UniversityNanning 530004China

Unraveling the essence of electronic structure effected by d-d orbital coupling of transition metal and methanol oxidation reaction(MOR)performance can fundamentally guide high efficient catalyst ***,density functional theory(DFT)calculations were performed at first to study the d–d orbital interaction of metallic Pt Pd Cu,revealing that the incorporation of Pd and Cu atoms into Pt system can enhance d-d electron interaction via capturing antibonding orbital electrons of Pt to fill the surrounding Pd and Cu *** the theoretical guidance,Pt Pd Cu medium entropy alloy aerogels(Pt Pd Cu MEAAs)catalysts have been designed and systematically screened for MOR under acid,alkaline and neutral ***,DFT calculation and in-situ fourier transform infrared spectroscopy analysis indicate that Pt Pd Cu MEAAs follow the direct pathway via formate as the reactive intermediate to be directly oxidized to CO_(2).For practical direct methanol fuel cells(DMFCs),the Pt Pd Cu MEAAs-integrated ultra-thin catalyst layer(4–5μm thickness)as anode exhibits higher peak power density of 35 m W/cm^(2) than commercial Pt/C of 20 m W/cm^(2)(~40μm thickness)under the similar noble metal loading and an impressive stability retention at a 50-m A/cm^(2) constant current for 10 *** work clearly proves that optimizing the intermediate adsorption capacity via d-d orbital coupling is an effective strategy to design highly efficient catalysts for DMFCs.

关键词： Medium-entropy alloys aerogels d-d Orbitals coupling pH-general Methanol oxidation reaction Ultra-thin catalyst layer

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Design, fabrication and performance test of an integrated exploding foil initiator system

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Defence technology（防务技术） 2024年第12期42卷 125-135页

作者： Zehao Wang Pengfei Xue Qingxuan Zeng Mingyu Li State Key Laboratory of Explosion Science and Technology Beijing Institute of TechnologyBeijing100081China Institute of Chemical Materials China Academy of Engineering PhysicsMianyang621900China

The integration method of exploding foil initiator system(EFIs) used to be researched to broaden its application range in military and aerospace in the last few *** order to lower the firing voltage below 1 kV,an integrated EFIs with enhanced energy efficiency was *** exploding foil initiator chips were fabricated in batch via micro electromechanical systems technology by integrating a unified foil,a flyer layer and a barrel on a glass substrate successively,meanwhile its package of the whole system was proposed at a volume of 2.194 cm^(3).The structural parameters were determined by predicted performance including flyer velocity,impact behavior and conduction property via the proposed theoretical models and the static electric field *** expect,this integrated EFIs exhibited excellent functions,which could accelerate the flyer to a terminal velocity over 4 km/s and preeminently initiate HNS-IV pellet at a circuit of 0.24 μF/0.9 ***,the theoretical design,fabrication and performance test have been all included to validate the feasibility of this integrated EFIs that was beneficial for its commercial development in the future.

关键词： Exploding foil initiator system Integration Planar trigger switch Micro electromechanical systems Flyer velocity Shock initiation

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chemical Synthesis of Globo H and Mannobiose Glycopolymers and their Immunological Stimulation

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Chinese Journal of Polymer Science 2024年第11期42卷 1661-1667,I0007页

作者： Zhi Zhang Ce-Ce Xue Ying-Le Feng Guo-Song Chen The State Key Laboratory of Molecular Engineering of Polymers and Department of Macromolecular Science Fudan UniversityShanghai200433China School of Chemistry and Chemical Engineering Shaanxi Normal UniversityXi’an710119China

Tumor-associated carbohydrate antigens(TACAs)provide a special class of tumor-specific antigens that show promising applications in cancer ***,the weak immunogenicity and structural complexity of TACAs are obstacles to their clinical ***,based on a fast and low-cost purification strategy for oligosaccharide synthesis,the synthesis of tumour-associated carbohydrate antigens Globo H and mannobiose which resembles repeat unit of mannan was *** enhance the immunogenicity and multivalent effect,Globo H and mannobiose were covalently attached to degradable polymer backbones.2D spindle-like lamellar micelle and globular micelle were obtained from glycopolymer through a solvent-exchange method of *** glyconanoparticle showed good biocompatibility and *** functions of these glyconanoparticles such as stimulation of BMDC to cause upregulation of inflammatory factors were preliminarily explored.

关键词： Globo-H Mannobiose Glycopolymer Convergent Synthesis Tumor-associated carbohydrate antigens

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Rapid velocity reduction and drift potential assessment of off-nozzle pesticide droplets

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Chinese Journal of chemical engineering 2022年第6期35卷 243-254页

作者： Shidong Xue Jingkun Han Xi Xi Junyi Zhao Zhong Lan Rongfu Wen Xuehu Ma Liaoning Key Laboratory of Clean Utilization of Chemical Resources Institute of Chemical EngineeringSchool of Chemical EngineeringDalian University of TechnologyDalian 116024China

The droplet velocity and diameter significantly affect both the spatial drift loss and the interfacial deposition behaviors, thus determining the ultimate utilization efficiency during pesticide *** the spatial velocity and diameter evolutions can reveal the mechanism of drift loss and guide to design regulation strategy. Here, we explored the spatial velocity distribution of droplets after leaving the nozzle by particle image velocimetry technology and particle tracking model, considering that the effect of nozzle configuration and the air velocity. It shows that all droplets decelerate rapidly with the velocity attenuation ratio ranging from 50% to 80% within the region of 200 mm below the *** spatial velocity evolution differences between droplets in crossflow are determined by the competition of vertical drag force and net gravity, and the drag force sharply increases as the droplet diameter decreases, especially for that smaller than 150 μm. Based on the spatial evolution differences of the droplet velocity and diameter, a functional adjuvant was added to the liquid for improving the diameter distribution. And the drift loss was significantly reduced due to the reduction of the proportion of easily drifting droplets.

关键词： Spray droplets Particle image velocimetry(PIV) Particle size distribution Multiphase flow Pesticide drift

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Progress in the design and performance evaluation of catalysts for low-temperature direct ammonia fuel cells

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Green chemical engineering 2025年第1期6卷 54-67页

作者： Zhongbin Gong Hao Wang Chenhao Li Qinqin Sang Ying Xie Xiaosa Zhang Yanrong Liu College of Science Shenyang University of Chemical TechnologyShenyang110142China CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Mesoscience and EngineeringBeijing Key Laboratory of Ionic Liquids Clean ProcessInstitute of Process EngineeringChinese Academy of SciencesBeijing100190China Longzihu New Energy Laboratory Zhengzhou Institute of Emerging Industrial TechnologyHenan UniversityZhengzhou450000China School of Chemical Engineering University of Chinese Academy of SciencesBeijing100049China

Ammonia,a hydrogen-rich and carbon-free energy carrier,possesses advantages such as high energy density and convenient liquefaction storage and serves as an optimal medium for hydrogen ***-temperature direct ammonia fuel cells(DAFCs)represent a highly promising pathway for the efficient utilization of ammonia ***,the sluggish kinetics of the low-temperature ammonia oxidation reaction(AOR),requires high loading of platinum-group metals(PGMs)catalysts,and their poisoning significantly hampers the performance of DAFCs,thereby limiting their large-scale commercial ***,it is crucial to design efficient,cost-effective,and stable *** this work,a detailed review of recent research efforts aimed at elucidating the mechanism underlying the AOR is *** on this knowledge base,progress in the design and synthesis of both PGM and PGM-free catalysts for the AOR is discussed,as well as membrane electrode assembly(MEA)preparation processes for ***,the results of the performance evaluation of AOR catalysts in single-cell tests are ***,based on our findings from this research area thus far,potential design strategies for AOR catalysts that can promote the rapid development of low temperatures DAFCs are proposed.

关键词： Low-temperature direct ammonia fuel cells Anti-poisoning ammonia oxidation catalysts Membrane electrode assembly Single-cell evaluation

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Layer stacked SiO_(x) microparticle with disconnected interstices enables stable interphase and particle integrity for lithium-ion batteries

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Journal of Energy Chemistry 2023年第11期86卷 300-307,I0007页

作者： Yang Ren Xucai Yin Lizhi Xiang Rang Xiao Hua Huo Geping Yin Chunyu Du MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage and Institute of Advanced Chemical Power Sources School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001HeilongjiangChina Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology School of Chemistry and Chemical EngineeringGuangxi UniversityNanning 530004GuangxiChina

Severe mechanical fractu re and unstable interphase,associated with the large volumetric expansion/contraction,significantly hinder the application of high-capacity SiO_(x)materials in lithium-ion ***,we report the design and facile synthesis of a layer stacked SiO_(x)microparticle(LS-SiO_(x))material,which presents a stacking structure of SiO_(x)layers with abundant disconnected *** LS-SiO_(x)microparticle can effectively accommodate the volume expansion,while ensuring negligible particle *** importantly,the interstices within SiO_(x)microparticle are disconnected from each other,which efficiently prevent the electrolyte from infiltration into the interior,achieving stable electrode/-electrolyte ***,the LS-SiO_(x)material without any coating delivers ultrahigh average Coulombic efficiency,outstanding cycling stability,and full-cell *** 6 cycles can attain>99.92%Coulombic efficiency and the capacity retention at 0.05 A g^(-1)for 100 cycles exceeds99%.After 800 cycles at 1 A g^(-1),the thickness swelling of LS-SiO_(x)electrode is as low as 0.87%.Moreover,the full cell with pure LS-SiO_(x)anode exhibits capacity retention of 91.2%after 300 cycles at 0.2 *** work provides a novel concept and effective approach to rationally design silicon-based and other electrode materials with huge volume variation for electrochemical energy storage applications.

关键词： Lithium-ion batteries Silicon oxide Layer stacked structure Disconnected interstices Coulombic efficiency

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Lithium-Sulfur Batteries at Extreme Temperatures:Challenges,Strategies and Prospects

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Energy & Environmental Materials 2023年第4期6卷 297-311页

作者： Wenjia Qu Jingyi Xia Chong Luo Chen Zhang Renjie Chen Wei Lv Quanhong Yang Nanoyang Group State Key Laboratory of Chemical EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Beijing Key Laboratory of Environmental Science and Engineering School of Material Science and EngineeringBeijing Institute of TechnologyBeijing 10081China School of Marine Science and Technology Tianjin UniversityTianjin 300072China Shenzhen Geim Graphene Center Engineering Laboratory for Functionalized Carbon MaterialsTsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055China

High-energy-density-batteries working at a wide-temperature range are urgently required in many performance-critical ***-sulfur batteries(LSB)are promising high-energy-density batteries that have the potential to maintain high performance at extreme ***,some problems like severe shuttling and safety issues at high temperatures or sluggish reaction kinetics and charge-transfer process at low temperatures decrease the performance and hinder their practical uses in extreme temperature ***,broadening the working temperature of LSB with stable electrochemical performance becomes a crucial *** this paper,the key stumbling blocks for high and low-temperature LSB are comprehensively *** solutions from the aspects of electrolyte and electrode materials are discussed to solve the aggravating shuttle effect and thermal safety issues under high temperature and the sluggish reaction kinetics under low ***,some specific promising solutions to extend the operating temperature range of LSB are also proposed and highlighted,which provide potential research directions on the practical LSB application in future.

关键词： high temperature lithium-sulfur batteries low temperature safety issue shuttle effect

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Viscosity-responsive signal amplification dual-modal probe triggered by cysteine/homocysteine for monitoring diabetic liver damages and repair processes

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Chinese chemical Letters 2025年第3期36卷 328-334页

作者： Sixin Ai Wenxiu Li Huayong Zhu Yang Wan Weiying Lin Institute of Optical Materials and Chemical Biology Guangxi Key Laboratory of Electrochemical Energy MaterialsSchool of Chemistry and Chemical EngineeringGuangxi UniversityNanning 530004China

Diabetic liver injury is a widespread complication of diabetes and carries a high risk to liver ***,early diagnosis of diabetic liver injury is of great significance for providing quality of life for diabetic *** of the activated dual-modal probes are usually activated by single factor stimulation,which greatly reduces the diagnostic accuracy of liver ***,a novel cysteine(Cys)/homocysteine(Hcy)and viscosity-enhanced dual-modal probe DAL was developed for the first time to monitor diabetic liver injury and its repair *** the presence of Cys/Hcy,the near-infrared fluorescence(NIRF)and photoacoustic(PA)signals of the probe DAL were activated,with further signal enhancement in high viscosity *** Cys/Hcy and viscosity cascade probe exhibits heightened sensitivity and enhanced anti-interference capabilities,contributing to the advancement of liver injury diagnosis *** addition,the probe DAL shows exceptional mitochondrial targeting ability,enabling sensitive monitoring of Cys/Hcy and viscosity alterations within *** on NIRF/PA dual-modal imaging technology,the probe was successfully used for the first time in a mouse diabetic liver injury model to evaluate the extent of liver damage and the repair process by tracking the levels of Cys/Hcy and ***,the two-factor activated dual-modal probe developed in this study provides a powerful instrument for accurate diagnosis and efficacy evaluation of complications related to diabetes.

关键词： Cysteine/homocysteine Viscosity responsive Near-infrared fluorescence Photoacoustic imaging Fluorescence imaging

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Interface engineering of Co nanoparticles decorated by Ir confined in N-doped carbon nanotubes for flexible Zn-air batteries and pH-universal overall water splitting

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Rare Metals 2024年第12期43卷 6447-6459页

作者： Ying-Gang Sun Xin Du Ji-Gang Wang Qiang Liu Jing-Lin Mu Zhong-Fang Li He-Qing Jiang Li-Kai Wang School of Chemistry and Chemical Engineering Shandong University of TechnologyZibo255049China School of Chemistry Zhengzhou UniversityZhengzhou450001China Qingdao Key Laboratory of Functional Membrane Material and Membrane Technology Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao266100China School of Chemical and Biological Engineering and Institute of Chemical ProcessSeoul National UniversitySeoul08826Korea

To alleviate the crisis of energy shortages,the scalable fabrication of highly efficient electrocatalysts is highly sought after for metal-air batteries and pH-universal overall water ***,an in situ construction to achieve Co@Ir nanoparticles in N-doped carbon nanotubes has been explored,which were directly fabricated by the pyrolysis and galvanic *** interface engineering of Co@Ir core-shell structures could enhance interfacial and synergistic effects,achieving the tailorable electrocatalytic activities for oxygen reduction reaction,oxygen evolution reaction and hydrogen evolution ***@Ir-NT demonstrates the outstanding stability for overall water splitting under pH-universal ***@Ir-NT-based r-ZABs display a high power density of295.1 mW·cm^(-2)and a ultralong cycle stability over 2000continuous charge-discharge cycles,and Co@Ir-NT-based F-ZABs maintain the similar performance at different bending angles,suggesting its promising potential in the application of wearable *** corresponding theoretical calculations also indicate that Co@Ir core-shell structure could improve the adsorption capacity and facilitate the breakage of O-O ***,this work might be helpful for developing multifunctional catalysts for metalair batteries and water splitting under pH-universal conditions.

关键词： Co@Ir Carbon nanotubes Electrocatalysts Zn-air batteries Water splitting

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Photoexcited singlet enhanced oxygen reduction reaction with high selectivity on the photosensitizer/layered double hydroxides nanocomposite

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Nano Research 2023年第4期16卷 5938-5945页

作者： Beibei Yang Sheng Tao Xuefei Liu Jun Lu State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China Tianjin University Tianjin 300072China

Oxygen reduction reaction(ORR)plays a pivotal role in advanced electrochemical energy conversion ***,the ORR conversion efficiency is extremely *** major obstacles originate from the adsorption and activation of O_(2)on the electrode surface.A novel nanocomposite catalyst,photosensitizers(PS)meso-tetraphenylporphyrin iron(III)chloride(FePcCl)/NiCoFe-layered double hydroxides(NiCoFe-LDHs)is designed in this ***,owing to excellent oxygen molecules activation ability and remarkable illumination absorption feature,FePcCl/NiCoFe-LDHs is employed to uncover the relationship between the intrinsic ORR activity and PS ***,the reaction mechanism of singlet 1O_(2)is proposed owing to the combination of electrochemical ORR catalysed via LDHs and *** boosted cathodic ORR properties exhibit singlet 1O_(2)dependent response arising from the synergistic effect to selectively produce active intermediates in alkaline *** work imparts the promising new mechanism about the high 4-electron ORR selectivity via material design,which will guide the development of photo-assisted energy conversion devices.

关键词： oxygen reduction reaction singlet 1O_(2) photosensitizers photo-assisted energy conversion layered double hydroxides

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