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Sub-10-nm-sized Au@AuxIr1-x metal-core/alloy-shell nanoparticles as highly durable catalysts for acidic water splitting

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National science Review 2024年第4期11卷 130-140页

作者： Huimin wang Zhe-ning chen Yuanyuan wang Dongshuang wu Minna cao Fanfei Sun Rong cao State Key laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences University of Chinese Academy of sciences School of Materials science and engineering Nanyang Technological University shanghai Synchrotron Radiation Facility Shanghai Institute of Applied Physics Chinese Academy of Sciences Fujian science & technology Innovation laboratory for Optoelectronic Information of china

The absence of efficient and durable catalysts for oxygen evolution reaction（OER） is the main obstacle to hydrogen production through water splitting in an acidic ele ***,we report a controllable synthesis method of surface IrOxwith changing Au/Ir compositions by constructing a range of sub-10-nm-sized core-shell nanocatalysts composed of an Au core and AuxIr1-xalloy *** particular,Au@Au0.43Ir0.57exhibits 4.5 times higher intrinsic OER activity than that of the commercial Ir/*** X-ray-based spectroscopies,electron microscopy and density functional theory calculations revealed a balanced binding of reaction intermediates with enhanced *** water-splitting cell using a load of 0.02 mgIr/cm2of Au@Au0.43Ir0.57as both anode and cathode can reach 10 mA/cm2at 1.52 V and maintain activity for at least194 h,which is better than the cell using the commercial couple Ir/C‖Pt/C（1.63 V,0.2 h）.

关键词： controllable synthesis of surface IrOx oxygen evolution reaction acidic water splitting catalytic stability transition metal catalysts

Microfluidic preparation of surfactant-free ultrafine DAAF with tunable particle size for insensitive initiator explosives

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Defence technology（防务技术） 2024年第9期39卷 42-52页

作者： Bo yang rui Li Wei cao Si-min He Jincan Zhu Qi wu Heng Ding Jin chen Weimiao wang Zhiqiang Qiao Xiaodong Li Guangcheng yang institute of Chemical Materials China Academy of Engineering PhysicsMianyang 621900China Southwest University of science and technology Mianyang 621010China School of Chemical engineering Nanjing University of Science and TechnologyNanjing 210094China

High purity and ultrafine DAAF(u-DAAF)is an emerging insensitive charge in *** there are many ways to obtain u-DAAF,developing a preparation method with stable operation,accurate control,good quality consistency,equipment miniaturization,and minimum manpower is an inevitable requirement to adapt to the current social technology development *** reported is the microfluidic preparation of u-DAAF with tunable particle size by a passive swirling *** the guidance of recrystallization growth kinetics and mixing behavior of fluids in the swirling microreactor,the key parameters(liquid flow rate,explosive concentration and crystallization temperature)were screened and optimized through screening *** the condition that no surfactant is added and only experimental parameters are controlled,the particle size of recrystallized DAAF can be adjusted from 98 nm to 785 nm,and the corresponding specific surface area is 8.45 m^(2)·g^(-1)to 1.33 m^(2)·g^(-1).In addition,the preparation method has good batch stability,high yield(90.8%-92.6%)and high purity(99.0%-99.4%),indicating a high practical application *** explosion derived flyer initiation tests demonstrate that the u-DAAF shows an initiation sensitivity much lower than that of the raw DAAF,and comparable to that of the refined DAAF by conventional spraying crystallization *** study provides an efficient method to fabricate u-DAAF with narrow particle size distribution and high reproducibility as well as a theoretical reference for fabrication of other ultrafine explosives.

关键词： Microfluidic preparation Screening crystallization conditions Narrow particle size distribution Low initiation sensitivity Ultrafine DAAF

Electronegativity-assisted optimized electronic structure of functionalized-Pt catalysts for boosting oxygen reduction kinetics

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Rare Metals 2024年第5期43卷 1965-1976页

作者： Jin Long Kai-Wen Zhuang Wei Liao Yan An Bin wang chen-Zhong wu Jian-Xin cao Qing wang Jun-Song chen Qing-Mei wang Guizhou University Key laboratory of Green Chemical and Clean Energy technology School of Chemistry and Chemical EngineeringGuizhou UniversityGuiyang 550025China Guizhou University engineering Research Center of Effcient Utilization for Industrial Waste Guizhou UniversityGuiyang 550025China institute of Dual-Carbon and New Energy technology Innovation and Development of Guizhou Province Guiyang 550025China Department of Dermatology West China HospitalSichuan UniversityChengdu610041China institute for Catalysis Hokkaido UniversitySapporo 001-0021Japan School of Materials and Energy University of Electronic Science and Technology of ChinaChengdu 611731China Interdisciplinary Materials Research Center Institute for Advanced StudyChengdu UniversityChengdu 610106China

Opportunity to harmonize aspects of oxygen reduction reaction(ORR)performance and structure,and morphology,as well as composition,is urgent for the commercialization of proton exchange membrane fuel ***,we demonstrate the design and synthesis of a functionalized-supported-Pt catalyst(Pt@HNC)featuring a hollow nitrogen-modified dodecahedral carbon substrate obtained by a stress-induced-shrink tailoring *** as-obtained Pt@HNC catalyst possesses enhanced ORR per-formance,in particular with half-wave potential,mass activity(MA)and specific activity,which greatly exceed the commercial Pt/*** density functional theory(DFT)calculations further confirmed that the charge redistribution induced by the electronegativity differences improved the electron interaction between Pt and HNC *** optimized electronic structure of Pt weakens the reaction energy barrier on the Pt@HNC surface and adsorption of^(*)OH species,thus cooperatively improving the intrinsic activity toward ***,our work indeed provides a guide for the future design of functional nanomaterials in the field of catalysts and clean energy.

关键词： Proton exchange membrane fuel cell(PEMFC) Oxygen reduction catalysis Supported Pt-based catalyst Stability

engineering FeOOH/Ni(OH)_(2) heterostructures on Ni_(3)S_(2)surface to enhance seawater splitting

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Rare Metals 2024年第5期43卷 1989-1998页

作者： chen yang Ya-Dong Li Li-Juan cao Xi-Long wang Han-Pu Liang Qingdao institute of Bioenergy and Bioprocess technology Chinese Academy of SciencesQingdao 266101China Center of Materials science and Optoelectronics engineering University of Chinese Academy of SciencesBeijing 100049China Sino-Danish College University of Chinese Academy of SciencesBeijing 100049China

The construction of highly stable and efficient electrocatalysts is desirable for seawater splitting but remains challenging due to the high concentration of Cl-in ***,FeOOH/Ni(OH)_(2)heterostructure supported on Ni_(3)S_(2)-covered nickel foam(Fe–Ni/Ni_(3)S_(2)/NF)was fabricated by hydrothermal and etching methods,as well as anodic oxidation *** electronic structure of FeOOH and Ni(OH)_(2)could be modulated after depositing FeOOH nanoparticles on Ni(OH)_(2)nanosheet,which greatly boosted the catalytic *** the catalyst used as an electrode for oxygen evolution reaction(OER),it needed low overpotentials of 266 and 368 m V to achieve current densities of 100 and 800 m A·cm^(-2),respectively,in 1 mol·L^(-1)KOH+seawater *** can operate continuously at 100 m A·cm^(-2)for 400 h without obvious ***,in situ generated SO_(4)^(2-)from inner Ni_(3)S_(2)during electrolysis process would accumulate on the surface of active sites to form passivation layers to repel Cl^(-),which seemed to be responsible for superior *** study not only synthesizes an OER catalyst for highly selective and stable seawater splitting,but also gives a novel approach for industrial hydrogen production.

关键词： Anodic oxidation Heterostructure Oxygen evolution reaction Seawater splitting

Ultra-thin robust CNT@GC film integrating effective electromagnetic shielding and flexible Joule heating

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Nano Research 2024年第5期17卷 3462-3471页

作者： Ding Zhang Chunhui wang Meng Li Weixue Meng Shipeng Zhang Mengdan yang Xinguang Huang Yingjiu Zhang Yuanyuan shang Anyuan cao Key laboratory of Materials physics(Ministry of Education) School of Physics and MicroelectronicsZhengzhou UniversityZhengzhou450052China Electron Microscopy Center Yunnan UniversityKunming650091China School of Materials science and engineering Peking UniversityBeijing100871China

The demand for lightweight,thin electromagnetic interference(EMI)shielding film materials with high shielding effectiveness(SE),excellent mechanical properties,and stability in complex environments is particularly pronounced in the realm of flexible and portable electronic ***,we developed an ultra-thin film(CNT@GC)in which the glassy carbon(GC)layer wrapped around and welded carbon nanotubes(CNTs)to form a core-shell network structure,leading to exceptional tensile strength(327.2 MPa)and electrical conductivity(2.87×10^(5) S·m^(−1)).The CNT@GC film achieved EMI SE of 60 dB at a thickness of 2µm after post-acid treatment and high specific SE of 3.49×10^(5) dB·cm^(2)·g^(−1),with comprehensive properties surpassing those of the majority of previous shielding ***,the CNT@GC film exhibited Joule heating capability,reaching a surface temperature of 135℃at 3 V with a fast thermal response of about 0.5 s,enabling anti-icing/de-icing *** work presented a methodology for constructing a robust CNT@GC film with high EMI shielding performance and exceptional Joule heating capability,demonstrating immense potential in wearable devices,defense,and aerospace applications.

关键词： core-shell structure ultra-thin lightweight film robust film electromagnetic shielding Joule heating

Bio-cementation for tidal erosion resistance improvement of foreshore slopes based on microbially induced magnesium and calcium precipitation

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Journal of Rock Mechanics and Geotechnical engineering 2024年第5期16卷 1696-1708页

作者： Xiaohao Sun Junjie wang Hengxing wang Linchang Miao Ziming cao Linyu wu institute of Geotechnical engineering Southeast UniversityNanjing211189China School of Civil engineering and Architecture Wuhan Polytechnic UniversityWuhan430070China

In most coastal and estuarine areas,tides easily cause surface erosion and even slope failure,resulting in severe land losses,deterioration of coastal infrastructure,and increased *** bio-cementation technique has been previously demonstrated to effectively improve the erosion resistance of *** contains magnesium ions(Mg^(2+))with a higher concentration than calcium ions(Ca^(2+));therefore,Mg^(2+)and Ca^(2+)were used together for bio-cementation in this study at various Mg^(2+)/Ca^(2+)ratios as the microbially induced magnesium and calcium precipitation(MIMCP)*** angles,surface strengths,precipitation contents,major phases,and microscopic characteristics of precipitation were used to evaluate the treatment *** showed that the MIMCP treatment markedly enhanced the erosion resistance of *** Mg^(2+)/Ca^(2+)ratios resulted in a smaller change in angles and fewer soil losses,especially the Mg^(2+)concentration below 0.2 *** decreased Mg^(2+)/Ca^(2+)ratio achieved increased precipitation contents,which contributed to better erosion resistance and higher surface ***,the production of aragonite would benefit from elevated Mg^(2+)concentrations and a higher Ca^(2+)concentration led to more nesquehonite in magnesium precipitation *** slopes with an initial angle of 53°had worse erosion resistance than the slopes with an initial angle of 35°,but the Mg^(2+)/Ca^(2+)ratios of 0.2:0.8,0.1:0.9,and 0:1.0 were effective for both slope stabilization and erosion mitigation to a great *** results are of great significance for the application of MIMCP to improve erosion resistance of foreshore slopes and the MIMCP technique has promising application potential in marine engineering.

关键词： Bio-cementation Erosion resistance Foreshore slope stabilization Magnesium ions Calcium ions

Construct a 3D microsphere of HMX/B/Al/PTFE to obtain the high energy and combustion reactivity

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Defence technology（防务技术） 2024年第2期32卷 45-54页

作者： Jian wang Jie chen Yaofeng Mao Yongjun Deng Wei cao Fude Nie Jun wang institute of Chemical Materials China Academy of Engineering PhysicsMianyang 621999PR China Shock and Vibration of engineering Materials and Structures Key Lab of Sichuan Province Mianyang 621010PR China

Metal(aluminum and boron)based energetic materials have been wildly applied in various fields including aerospace,explosives and micro-devices due to their high energy ***,the low combustion efficiency and reactivity of metal fuels,especially boron(B),severely limit their practical ***,multi-component 3D microspheres of HMX/B/Al/PTFE(HBA)have been designed and successfully prepared by emulsion and solvent evaporation method to achieve superior energy and combustion *** reactivity and energy output of HBA are systematically measured by ignitionburning test,constant-volume explosion vessel system and bomb *** to the increased interfacial contact and reaction area,HBA shows higher flame propagation rate,faster pressurization rate and larger combustion heat of 29.95 cm/s,1077 kPa/s,and 6164.43 J/g,which is 1.5 times,3.5 times,and 1.03 times of the physical mixed counterpart(HBA-P).Meanwhile,HBA also shows enhanced energy output and reactivity than 3D microspheres of HMX/B/PTFE(HB)resulting from the high reactivity of *** reaction mechanism of 3D microspheres is comprehensively investigated through combustion emission spectral and thermal analysis(TG-DSC-MS).The superior reactivity and energy of HBA originate from the surface etching of fluorine to the inert shell(Al_(2)O_(3) and B_(2)O_(3))and the initiation effect of Al to *** work offers a promising approach to design and prepare high-performance energetic materials for the practical applications.

关键词： HMX/B/Al/PTFE 3D microspheres surface etching Reaction mechanism

Atomistic origin of high grain boundary resistance in solid electrolyte lanthanum lithium titanate

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Journal of Materiomics 2024年第6期10卷 1214-1221页

作者： shang Peng Yongjin chen Xuefeng Zhou Mingxue Tang Jianbo wang Hua wang Lin Guo Lujun Huang Wenge yang Xiang Gao Center for High Pressure science and technology Advanced Research(HPSTAR) Beijing100094China School of physics and technology Center for Electron MicroscopyMOE Key Laboratory of Artificial Micro-and Nano-structuresand Institute for Advanced StudiesWuhan UniversityWuhan430072China School of Chemistry Beijing Advanced Innovation Center for Biomedical EngineeringBeihang UniversityBeijing100191China School of Materials science and engineering Harbin Institute of TechnologyP.O.Box 433Harbin150001China

Lanthanum lithium titanate is one of the promising electrolytes for solid-state lithium-ion batteries due to its high bulk ionic conductivity up to∼10^(−3) S/***,the practical application of this material has been bottlenecked by high grain boundary(GB)resistance,while the underlying mechanism is still under *** we report a comprehensive study with direct evidence to reveal the origin of high GB resistance in La_(2/3)–xLi_(3x)TiO_(3)(LLTO).Atomic-scale observations via advanced scanning transmission electron microscopy show that the GBs are uniformly subject to subsurface segregation of La atoms to compensate for the excess surface *** La segregation leads to an abrupt decrease of charge carrier concentration neighboring GBs and hence is supposed to have deleterious effect on GB *** findings suggest a novel mechanism of space-charge-induced cation segregation,which shed lights on the intrinsic origin of low GB ionic conductivity in LLTO.

关键词： Space-charge layer Cation segregation Intergranullar glassy film Solid-state electrolyte Ionic conductivity

Efficient construction of calcium fluoride nanoaggregates for enhanced water vapor adsorption

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Particuology 2024年第6期89卷 191-197页

作者： Dan-Lei yang Jing cao Rong-Kun Liu Jie-Xin wang School of Life sciences and Chemical engineering Jiangsu Second Normal UniversityNanjing210013China State Key laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China Research Center of the Ministry of Education for High Gravity engineering and technology Beijing University of Chemical TechnologyBeijing100029China Petrochemical Research institute PetroChinaBeijing102206China

Calcium fluoride(CaF_(2))is an ideal adsorbent for the dehydration of gaseous hydrogen fluoride(HF)containing water *** this work,a novel CaF_(2)absorbent,spherical CaF_(2)nanoaggregates(NAs)with a closely packed structure,was proposed and efficiently fabricated by spray drying *** the building blocks of CaF_(2)NAs,the CaF_(2)nanoparticles(NPs)were prepared by the addition of excess calcium ions(Ca^(2+))or fluorine ions(F−)in the *** results indicated that the CaF_(2)NPs synthesized by excess Ca^(2+)and the corresponding NAs exhibited much better water vapor adsorption properties than their counterparts by excess F−,owing to higher zeta *** importantly,whether excess Ca^(2+)or F^(−),CaF_(2)NAs had further enhanced water vapor adsorption capacity compared to primary CaF_(2)NPs,possibly owing to their unique nano-micro secondary structures and higher surface *** work has great potential in the development of high-performance absorbents for separating moisture from corrosive gas HF.

关键词： CaF_(2)nanoaggregates Water vapor adsorption Spray drying