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Synergistic integration of self-supported 1T/2H-WS_(2) and nitrogendoped rGO on carbon cloth for pH-universal electrocatalytic hydrogen evolution

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Nano research 2024年第3期17卷 1267-1280页

作者： Feng Ming Yap Jian Yiing Loh Wee-Jun Ong School of Energy and chemical Engineering Xiamen University MalaysiaSelangor Darul Ehsan 43900Malaysia Center of Excellence for NaNo Energy&Catalysis Technology(CONNECT) Xiamen University MalaysiaSelangor Darul Ehsan 43900Malaysia State Key Laboratory of physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Gulei Innovation institute Xiamen UniversityZhangzhou 363200China Shenzhen research institute of Xiamen University Shenzhen 518057China

Hydrogen economy based on electrochemical water splitting exemplified one of the most promising means for overcoming the rapid consumption of fossil fuels and the serious deterioration of global *** development of earth-abundant,efficient,and durable electrocatalysts for hydrogen evolution reaction(HER)plays a vital role in the commercialization of water ***,the self-supported electrode with unique nitrogen-doped reduced graphene oxide(N-rGO)nanoflakes and WS_(2) hierarchical nanoflower that were grown directly on carbon cloth(CC)substrate(WS_(2)/N-rGO/CC)was successfully synthesized using a facile dual-step hydrothermal *** as-synthesized 50%1T/2H-WS_(2)/N-rGO/CC(WGC),which possessed high metallic 1T phase of 57%not only efficiently exposed more active sites and accelerated mass/charge diffusion,but also endowed excellent structural lustiness,robust stability,and durability at a high current *** a result,the 50%WGC exhibited lower overpotentials and Tafel slopes of 21.13 mV(29.55 mV∙dec^(-1))and 80.35 mV(137.02 mV∙dec^(-1))as compared to 20%Pt-C/CC,respectively for catalyzing acidic and alkaline hydrogen evolution ***,the as-synthesized 50%WGC also depicted long-term stability for more than 8 h in the high-current-density regions(100 and 220 mA∙cm^(-2)).In brief,this work reveals a self-supported electrode as an extraordinary alternative to Pt-based catalysts for HER in a wide pH range,while paving a facile strategy to develop advanced electrocatalysts with abundant heterointerfaces for practical applications in energy-saving hydrogen production.

关键词： self-supported electrocatalyst carbon-based substrate phase engineering pH-universal water splitting

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Local environment regulation of transition metal dichalcogenide-based single-atom catalysts

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Rare Metals 2024年第9期43卷 4019-4037页

作者： Ming-Hui Li Jing Li Xiao-Yu Zheng Yao Zhou Advanced research institute of Multidisciplinary Science and School of Chemistry and chemical Engineering Beijing Institute of TechnologyBeijing 100081China Laser Micro/Nano Fabrication Laboratory School of Mechanical EngineeringBeijing Institute of TechnologyBeijing 100081China

Single-atom catalysts have risen significant attention in the realm of green electrocatalytic energy conversion to address energy and environmental sustainability *** metal dichalcogenide(TMD)-based single-atom catalysts are considered highly effective in electrocatalysis due to the TMDs'notable specific surface area,tunable elemental species and efficient utilization of single *** order to enhance electrocatalytic performance,it is imperative to elaborately engineer the local environment surrounding the active sites of single atoms within *** this review,we initially explore the effects of synthesis methods on single-atom active sites and the influence of loading of single atoms on catalytic performance for *** modulation strategies of the local environment surrounding single-atom sites in TMDs are elaborated,including substitution engineering,surface adsorption,vacancies,spatial confinement and dual-atom site *** each modulation strategy,the effects of diverse local environments on various electrocatalytic applications are presented,such as the oxygen evolution reaction,oxygen reduction reaction,nitrogen reduction reaction,CO_(2)reduction reaction and CO ***,this study presents a comprehensive overview of the challenges encountered and the potential directions for the advancement of single-atom catalysts based on TMDs in the realm of electrocatalysis.

关键词： Single-atom catalysts Transition metal dichalcogenide Local environment Electrocatalysis

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Tandem hydroformylation/hydrogenation of olefins to alcohols using atomically dispersed bifunctional catalysts

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Science China Chemistry 2024年第11期67卷 3706-3711页

作者： Ying Zhang Liyang Liu Ziyue Wang Xingcong Zhang Xiaohui He Hongbing Ji Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education Fine Chemical Industry Research InstituteSchool of Chemistry IGCME Sun Yat-sen University Guangdong Technology research Center for Synthesis and Separation of Thermosensitive chemicals State Key Laboratory Breeding Base of Green-chemical Synthesis Technology Institute of Green Petroleum Processing and Light Hydrocarbon Conversion College of Chemical Engineering Zhejiang University of Technology

Tandem hydroformylation/hydrogenation of olefins to alcohols is an appealing and challenging route that has received continuous interest. Herein, we report a bifunctional atomically dispersed Rh and Co catalyst（Rh Co/Al2O3-10） prepared by a simple ball milling method that displays superior synergistic catalytic performance（>95% olefins conversion and >80% alcohols selectivity） and broad substrate scope for tandem hydroformylation/hydrogenation reaction, outperforming Rh/Al2O3, Co/Al2O3,and their physically mixed counterparts. In situ CO-DRIFTS, XPS, and kinetic experiments demonstrate that the electron interaction between Rh and Co atoms effectively lowers the apparent activation energy, thus promoting the tandem hydroformylation/hydrogenation reaction. This work not only presents a novel tandem hydroformylation/hydrogenation reaction system for converting olefins to alcohol but also throws light on the rational design of versatile bifunctional catalysts for ondemand synergistic catalysis.

关键词： tandem hydroformylation/hydrogenation alcohols bifunctional single atom catalysts

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Facet effects on bimetallic ZnSn hydroxide microcrystals for selective electrochemical CO2 reduction

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Green Energy & Environment 2024年第8期9卷 1314-1320页

作者： Liu Han Cheng-wei Wang Shan-shan Luo Ying-tang Zhou Bing Li Ming Liu School of Chemistry and chemical Engineering Harbin Institute of Technology National Engineering research Center for Marine Aquaculture Marine Science and Technology CollegeZhejiang Ocean University

Employing crystal facets to regulate the catalytic properties in electrocatalytic carbon dioxide reduction reaction（eCO2RR） has been well demonstrated on electrocatalysts containing single metals but rarely explored for bimetallic systems. Here, we synthesize Zn Sn（OH）6（ZSO）microcrystals（MCs） with distinct facets and investigate the facet effects in eCO2RR. Electrochemical studies and in situ Fourier Transform Infrared Spectroscopy（in situ-FTIR） reveal that ZSO MCs produce mainly C1 products of HCOOH and CO. The {111} facet of the ZSO MCS exhibits higher selectivity and faradaic efficiency（FE） than that of the {100} facet over a wide range of potentials（-0.9 V ～-1.3 V versus RHE）. Density Functional Theory（DFT） calculations elucidate that the {111} facet is favorable to the adsorption/activation of CO2molecules,the formation of intermediate in the rate-determining step, and the desorption of C1 products of CO and HCOOH molecules.

关键词： ZnSn(OH) 6 Crystal facets Electrochemical carbon dioxide reduction C1 product Density functional theory

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Single-atom-mediated electron islands boost photocatalytic CO_(2)chemical fixation

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Science China Chemistry 2024年第7期67卷 2292-2299页

作者： Shu Shang Lei Li Xin He Hui Wang Lirong Zheng Wei Shao Xiaodong Zhang Yi Xie Hefei National research Center for physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026China institute of Energy Hefei Comprehensive National Science CenterHefei 230031China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China School of Chemistry and chemical Engineering Hefei Normal UniversityHefei 230031China

Photocatalytic cycloadditions of CO_(2)with epoxides are emerging as a significant platform for the green synthesis of valuable carbonates,where efficient catalytic systems with spatially separated charge carriers are ***,a single p-block metal atom is proposed to be a candidate for photogenerated electron localization on a metal oxide *** taking the Bi single-atom supported on ZnO nanosheet(Bi1/ZnO)as an example,we show that the Bi atom plays the role of an electron island in the sea of delocalized holes within ***,the as-formed electron island could readily promote the rate-determining ring-opening process of cycloaddition *** from the unique spatially separated electrons and holes,the Bi1/ZnO achieves a high yield of cyclic carbonates with almost 100%*** study provides a pioneering strategy for enhancing the performances of photocatalytic CO_(2)chemical fixation.

关键词： electron islands CO_(2)photofixation photogenerated charge carriers

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High temperature deformation and recrystallization behavior of magnesium bicrystals with 90°<1010>and 90°<1120>tilt grain boundaries

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Journal of Magnesium and Alloys 2024年第2期12卷 625-638页

作者： Kevin Bissa Talal Al-Samman Dmitri A.Molodov institute of physical Metallurgy and Materials Physics RWTH Aachen University52056 AachenGermany International research Organization for Advanced Science and Technology(IROAST) Kumamoto UniversityKumamoto 860-8555Japan

The deformation mechanisms and dynamic recrystallization(DRX)behavior of specifically grown bicrystals with a symmetric 90°and 90°tilt grain boundary,respectively,were investigated under deformation in plane strain compression at 200℃and 400℃.The microstructures were analyzed by panoramic optical microscopy and large-area electron backscatter diffraction(EBSD)orientation *** analysis employed a meticulous approach utilizing hundreds of individual,small EBSD maps with a small step size that were stitched together to provide comprehensive access to orientation and misorientation data on a macroscopic *** slip primarily governed the early stages of deformation at the two temperatures,and the resulting shear induced lattice rotation around the transverse direction(TD)of the *** existence of the grain boundary gave rise to dislocation pile-up in its vicinity,leading to much larger TD-lattice rotations within the boundary region compared to the *** increasing temperature,the deformation was generally more uniform towards the bulk due to enhanced dislocation mobility and more uniform stress *** recrystallization at 200℃was initiated in{1011}-compression twins at strains of 40%and *** 400℃,DRX consumed the entire grain boundary region and gradually replaced the deformed microstructure with progressing *** recrystallized grains displayed characteristic orientations,such that their c-axes were perpendicular to the TD and additionally scattered between 0°and 60°from the loading *** recrystallized grains displayed mutual rotations of up to 30°around the c-axes of the initial grains,forming a discernible basal fiber texture component,prominently visible in the{1120}pole *** is noteworthy that the deformation and DRX behaviors of the two analyzed bicrystals exhibited marginal variations in response to strain and deformation temperature.

关键词： Elevated deformation temperatures Plain strain compression Magnesium bicrystals Panorama EBSD Dynamic Recrystallization

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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

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Investigation of system parameters towards safer impact based shock-to-detonation transition in a novel laser driven flyer plate prototype

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Defence Technology（防务技术） 2024年第9期39卷 103-113页

作者： Gonca Saglam Ozkasapoglu Selis Onel institute of Science Hacettepe UniversityBeytepe06800Turkey TUBITAK SAGE Defense Industries research and Development institute Ankara06261Turkey Department of chemical Engineering Hacettepe UniversityBeytepe06800AnkaraTurkey

Laser driven flyer plate technology offers improved safety and reliability for detonation of explosives in industrial applications ranging from mining and stone quarrying to the aerospace and defense *** study is based on developing a safer laser driven flyer plate prototype comprised of a laser initiator and a flyer plate subsystem that can be used with secondary *** parameters were optimized to initiate the shock-to-detonation transition(SDT)of a secondary explosive based on the impact created by the flyer plate on the explosive *** of the flyer was investigated at the mechanically weakened region located on the interface of these subsystems,where the product gases from the deflagration of the explosive provide the required energy.A bilayer energetic material was used,where the first layer consisted of a pyrotechnic component,zirconium potassium perchlorate(ZPP),for sustaining the ignition by the laser beam and the second layer consisted of an insensitive explosive,cyclotetramethylene-tetranitramine(HMX),for deflagration.A plexiglass interface was used to enfold the energetic *** focal length of the laser beam from the diode was optimized to provide a homogeneous beam profile with maximum power at the surface of the *** bomb experiments were conducted in an internal volume of 10 cm^(3) for evaluation of *** of the laser driven flyer plate system output on confinement,explosive density,and laser beam power were *** using a high-speed camera resulted in a flyer velocity of 670±20 m/s that renders the prototype suitable as a laser detonator in applications,where controlled employment of explosives is critical.

关键词： Laser driven flyer plate Shock to detonation transition Detonation Secondary explosives Pyrotechnic materials Confinement

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Enhanced direct gaseous CO_(2) fixation into higher bio-succinic acid production and selectivity

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Journal of Environmental Sciences 2024年第9期143卷 164-175页

作者： Ziyi Yang Wanling Wu Qing Zhao Irini Angelidaki Samuel Gyebi Arhin Dongliang Hua Yuxiao Zhao Hangyu Sun Guangqing Liu Wen Wang Biomass Energy and Environmental Engineering research Center Beijing University of Chemical TechnologyBeijing 100029China College of chemical Engineering Beijing University of Chemical TechnologyBeijing 100029China Department of chemical and Biochemical Environmental Engineering Technical University of DenmarkDK-2800Kgs LyngbyDenmark Energy research institute Qilu University of Technology(Shandong Academy of Sciences)Shandong Provincial Key Laboratory of Biomass Gasification TechnologyJinan 250014China

Utilizing CO_(2)for bio-succinic acid production is an attractive approach to achieve carbon capture and recycling(CCR)with simultaneous production of a useful platform *** succinogenes and Basfia succiniciproducens were selected and investigated as microbial ***,the type and concentration of inorganic carbon concentration and glucose concentration were evaluated.6 g C/L MgCO_(3)and 24 g C/L glucose were found to be the optimal basic operational conditions,with succinic acid production and carbon yield of over 30 g/L and over 40%,***,for maximum gaseous CO_(2)fixation,carbonate was replaced with CO_(2)at different ***“less carbonate more CO_(2)”condition of the inorganic carbon source was set as carbonate:CO_(2)=1:9(based on the mass of carbon).This condition presented the highest availability of CO_(2)by well-balanced chemical reaction equilibrium and phase equilibrium,showing the best performance with regarding CO_(2)fixation(about 15 mg C/(L·hr)),with suppressed lactic acid *** to key enzymes analysis,the ratio of phosphoenolpyruvate carboxykinase to lactic dehydrogenase was enhanced at high ratios of gaseous CO_(2),which could promote glucose conversion through the succinic acid *** further increase gaseous CO_(2)fixation and succinic acid production and selectivity,stepwise CO_(2)addition was evaluated.50%-65%increase in inorganic carbon utilization was obtained coupled with 20%-30%increase in succinic acid *** was due to the promotion of the succinic acid branch of the glucose metabolism,while suppressing the pyruvate branch,along with the inhibition on the conversion from glucose to lactic acid.

关键词： Succinic acid CO_(2) fixation Actinobacillus succinogenes Basfia succiniciproducens Lactic acid

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Antifouling Properties of Electrospun Polymeric Coatings Induced by Controlled Surface Morphology

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Energy & Environmental Materials 2024年第6期7卷 409-419页

作者： Fabio L.Favrin Lorenzo Zavagna Matteo Sestini Semih Esin Bahareh Azimi Massimiliano Labardi Mario Milazzo Giuseppe Gallone Giovanna Batoni Serena Danti Department of Civil and Industrial Engineering University of PisaLargo Lucio Lazzarino 256122PisaItaly Department of Translational research and New Technologies in Medicine and Surgery University of Pisavia San Zeno 35-3956123PisaItaly institute for chemical and physical Processes(IPCF) National Research Council(CNR)Pisa Research AreaVia Moruzzi 156124PisaItaly Department of Civil and Environmental Engineering Massachusetts Institute of Technology(MIT)Massachusetts Ave.77CambridgeMassachusetts 02139USA

Nosocomial infections affect implanted medical devices and greatly challenge their functional outcomes,becoming sometimes life threatening for the ***,aggressive antibiotic therapies are administered,which often require the use of last-resort drugs,if the infection is caused by multi-drug-resistant *** the risk of bacterial contamination of medical devices in the hospitals has thus become an emerging *** routes to control these infections are based on materials provided with intrinsic bactericidal properties(i.e.,chemical action)and on the design of surface coatings able to limit bacteria adhesion and fouling phenomena(i.e.,physical action),thus preventing bacterial biofilm ***,we report the development and validation of coatings made of layer-by-layer deposition of electrospun poly(vinylidene fluoride-co-trifluoro ethylene)P(VDF-TrFE)fibers with controlled orientations,which ultimately gave rise to antifouling *** obtained 10-layer surface morphology with 90°orientation fibers was able to efficiently prevent the adhesion of bacteria,by establishing a superhydrophobic-like behavior compatible with the Cassie-Baxter ***,the results highlighted that surface wettability and bacteria adhesion could be controlled using fibers with diameter comparable to bacteria size(i.e.,achievable via electrospinning process),by tuning the intra-fiber spacing,with relevant implications in the future design of biomedical surface coatings.

关键词： additive manufacturing Escherichia coli fibers Poly(vinylidene fluoride-cotrifluoro ethylene)P(VDF-TrFE) Pseudomonas aeruginosa superhydrophobic

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