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Deciphering dynamic surface of PtRu alloy nanocatalysts to revisit their synergistic effects during the electrooxidation

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Science China Chemistry 2024年第7期67卷 2224-2233页

作者： Xiao-Chong Li Bo Wang zhou Yu Qiang Wan Ju-Fang Zheng Emmanuel Maisonhaute Xiao-Shun zhou ya-Hao Wang Key Laboratory of the Ministry of Education for Advanced Catalysis Materials Institute of Physical ChemistryZhejiang Normal UniversityJinhua 321004China Laboratoire Interface et Systèmes Electrochimiques CNRS UMR 8235Sorbonne UniversitéF-75252 Paris cedex 5France

Correlating dynamic structural transformation of catalysts with the surface intermediate species under operating conditions is critical for updating the understanding of structure–performance ***,we probe the electrochemical potentialdependent surface structures and adsorbed intermediates on PtRu binary alloy nanocatalysts to revisit its synergistic mechanisms for CO electrooxidation enhanced ***-situ spectral characteristics by using modified shell-isolated nanoparticle-enhanced Raman spectroscopy,show that in acidic solution,when the potential is positively scanned from 0.1 V to 1.5 V relative to reversible hydrogen electrode(RHE),the surface of the alloy catalyst evolves from metallic PtRu to adsorbed oxygen gradually covering and accumulating on Ru sites(denoted as PtRuO_(x),x≤2),forming segregated RuO_(2),and finally forming a threedimensional oxide layer(denoted as 3D PtRuO_(4)).Moreover,molecular evidence associated with periodic density functional theory calculations reveals that electronic effects promote ruthenium to become more oxidizable and *** particular,we found here that ^(*)O and ^(*)OH at surface RuO_(x) sites are highly efficient CO oxidation active species in comparison to the same entities adsorbed on metallic Ru *** work sheds light on the complex surface dynamic process of practical Pt-based binary nanocatalysts and improves the understanding of synergistic mechanism for the development of fuel cell devices.

关键词： in-situ Raman spectroscopy surface evolution bifunctional mechanism PtRu electrooxidation

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Active Cu and Fe Nanoparticles Codecorated Ruddlesden-Popper-Type Perovskite as Solid Oxide Electrolysis Cells Cathode for CO2 Splitting

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Energy & Environmental Materials 2024年第5期7卷 219-227页

作者： Dongliang Liu Hang Shang chuan zhou Jie Miao Daxiang Xue Zeping Chen Meijuan Fei Fengli Liang Qiang Niu Ran Ran Wei zhou Zongping Shao State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical Engineering Nanjing Tech University Suzhou Laboratory School of Environmental Science and Engineering Nanjing Tech University Inner Mongolia Erdos Electric Power and Metallurgy Group Co. Ltd. Jiangsu Province Key Laboratory of Aerospace Power System College of Energy and Power Engineering Nanjing University of Aeronautics and Astronautics WA School of Mines: Minerals Energy and Chemical Engineering (WASM-MECE) Curtin University

Solid oxide electrolysis cells （SOECs）, displaying high current density and energy efficiency, have been proven to be an effective technique to electrochemically reduce CO2into CO. However, the insufficiency of cathode activity and stability is a tricky problem to be addressed for SOECs. Hence, it is urgent to develop suitable cathode materials with excellent catalytic activity and stability for further practical application of SOECs. Herein, a reduced perovskite oxide, Pr0.35Sr0.6Fe0.7Cu0.2Mo0.1O3-δ（PSFCM0.35）, is developed as SOECs cathode to electrolyze CO2. After reduction in 10%H2/Ar, Cu and Fe nanoparticles are exsolved from the PSFCM0.35 lattice,resulting in a phase transformation from cubic perovskite to Ruddlesden–Popper （RP） perovskite with more oxygen vacancies. The exsolved metal nanoparticles are tightly attached to the perovskite substrate and afford more active sites to accelerate CO2adsorption and dissociation on the cathode surface. The significantly strengthened CO2adsorption capacity obtained after reduction is demonstrated by in situ Fourier transforminfrared（FT-IR） spectra. Symmetric cells with the reduced PSFCM0.35 （RPSFCM0.35）electrode exhibit a low polarization resistance of 0.43Ωcm2at850℃. Single electrolysis cells with the R-PSFCM0.35 cathode display an outstanding current density of 2947 mA cm-2at 850℃and 1.6 V. In addition, the catalytic stability of the R-PSFCM0.35 cathode is also proved by operating at 800℃with an applied constant current density of600 mA cm-2for 100 h.

关键词： cathode CO2 reduction nanoparticles decoration solid oxide electrolysis cells

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Confinement of Fe atoms between MoS_(2) interlayers drives phase transition for improved reactivity in Fenton-like reactions

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Nano Research 2024年第3期17卷 1132-1139页

作者： Yibing Sun Yu zhou Hongchao Li chuan Wang Xuan Zhang Qian Ma Yingchun Cheng Jieshu Qian Bingcai Pan Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse School of Environmental and Biological EngineeringNanjing University of Science and TechnologyNanjing 210094China Key Laboratory of Flexible Electronics and Institute of Advanced Materials Jiangsu National Synergetic Innovation Center for Advanced MaterialsNanjing Tech UniversityNanjing 211816China Department of General Dentistry Affiliated Stomatological Hospital of Nanjing Medical UniversityJiangsu Province Key Laboratory of Oral DiseasesNanjing 210029China Research Center for Environmental Nanotechnology(ReCENT) State Key Laboratory of Pollution Control and Resources ReuseSchool of EnvironmentNanjing UniversityNanjing 210023China

Phase manipulation of MoS_(2) from thermodynamically stable 2H phase to the unstable but more reactive 1T phase represents a crucial strategy for improving the reactivity in many *** widely adopted wet chemistry approach uses intercalating entities especially alkali metal ions to achieve the phase transition;however,these entities are normally inert for the target ***,we describe the first use of iron atoms for the intercalation of 2H-MoS_(2) layers,driving the partial transition from 2H to 1T ***,in the peroxymonosulfate(PMS)-based Fenton-like reactions,the interlayered confinement of Fe atoms not only activates the inert basal plane,but also adds more reactive Fe sites for the formation of metal-PMS complex as primary reactive species for pollutant *** the degradation of a model pollutant carbamazepine(CBZ),the Fe-intercalated MoS_(2) exhibits a first order rate constant 13.3 times higher than 2H-MoS_(2).This strategy is a new direction for manipulating the phase composition and boosting the catalytic reactivity of MoS_(2)-based catalysts in various scenarios,including environmental remediation and energy applications.

关键词： confinement MoS_(2) Fe atoms Fenton-like reactions hydrogen evolution reaction

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Isorhamnetin Downregulates MMP2 and MMP9 to Inhibit Development of Rheumatoid Arthritis through SRC/ERK/CREB Pathway

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Chinese Journal of Integrative Medicine 2024年第4期30卷 299-310页

作者： LIU Xiao-rong LI Shuo-fu MEI Wen-ya LIU Xiang-dan zhou Ri-bao College of Pharmacy Hunan University of Chinese MedicineChangsha(410208)China Department of Orthopaedics The First Hospital of Hunan University of Chinese MedicineChangsha(410007)China

Objective To investigate the effect of isorhamnetin on the pathology of rheumatoid arthritis(RA).Methods Tumor necrosis factor(TNF)-α-induced fibroblast-like synoviocytes(FLS)was exposed to additional isorhamnetin(10,20 and 40µmol/L).Overexpression vectors for matrix metalloproteinase-2(MMP2)or MMP9 or SRC were transfected to explore their roles in isorhamnetin-mediated RA-FLS ***-FLS viability,migration,and invasion were ***,a collagen-induced arthritis(CIA)rat model was *** were randomly divided to sham,CIA,low-,medium-,and high-dosage groups using a random number table(n=5 in each group)and administed with normal saline or additional isorhamnetin[2,10,and 20 mg/(kg·day)]for 4 weeks,*** index was calculated and synovial tissue inflammation was determined in CIA *** levels of MMP2,MMP9,TNF-α,interleukin-6(IL-6),and IL-1β,as well as the phosphorylation levels of SRC,extracellular regulated kinase(ERK),and cyclic adenosine monophosphate response element-binding(CREB),were detected in RA-FLS and synovial *** docking was also used to analyze the binding of isorhamnetin to *** In in vitro studies,isorhamnetin inhibited RA-FLS viability,migration and invasion(P<0.05).Isorhamnetin downregulated the levels of MMP2,MMP9,TNF-α,IL-6,and IL-1βin RA-FLS(P<0.05).The overexpression of either MMP2 or MMP9 reversed isorhamnetin-inhibited RA-FLS migration and invasion,as well as the levels of TNF-α,IL-6,and IL-1β(P<0.05).Furthermore,isorhamnetin bound to SRC and reduced the phosphorylation of SRC,ERK,and CREB(P<0.05).SRC overexpression reversed the inhibitory effect of isorhamnetin on RA-FLS viability,migration and invasion,as well as the negative regulation of MMP2 and MMP9(P<0.05).In in vivo studies,isorhamnetin decreased arthritis index scores(P<0.05)and alleviated synovial *** reduced the levels of MMP2,MMP9,TNF-α,IL-6,and IL-1β,as well as the phosphorylation of SRC,ERK,and CRE

关键词： rheumatoid arthritis isorhamnetin SRC/ERK/CREB matrix metalloproteinase

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Two-dimensional silica enhanced solid polymer electrolyte for lithium metal batteries

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Particuology 2024年第2期85卷 146-154页

作者： Zhihong Luo Weiyong Li Chong Guo ya Song Mingxia zhou yan Shi Jing Xu Long Li Bin Shi Quansheng Ouyang Jiao-jing Shao Guangmin zhou School of Materials and Metallurgy Guizhou UniversityGuiyang550025China State Key Laboratory of Advanced Chemical Power Sources Zunyi563003China Graphene Materials Engineering Research Center of Guizhou Colleges and Universities Guiyang550025China Tsinghua-Berkeley Shenzhen Institute&Tsinghua Shenzhen International Graduate Schoo Tsinghua UniversityShenzhen518055China

Solid polymer electrolytes(SPEs)are promising substitutes for current flammable liquid electrolytes to achieve high-safety and high-energy-density lithium metal *** oxide(PEO)based solid polymer electrolytes have attracted increasing attention because of their excellent flexibility,manufacturability,light weight,and low-cost processing,while they often suffer from low ionic con-ductivity at room temperature,low lithium transference number and unsatisfactory interfacial resis-tance,which largely restrain their practical ***,two-dimensional holey silica nanosheets(2D-HSN)as the fillers,together with LiNO_(3) as the electrolyte additive,are introduced in a PEO/poly(-vinylidene fiuoride-co-hexafluoropropylene)(PVDF-HFP)blended polymer matrix to obtain a *** incorporation of HSN filler creates supplementary channels for lithium ion migration and lowers the crystallinity of the polymer,thereby facilitating the movement of lithium *** HSN-based SPE demonstrates higher ionic conductivity up to 3.7 x 10-4 S cm-1 at 30℃,larger Li+transference number close to 0.34,and more stable lithium plating/stripping than that without the fillers,and HSN can promote the formation of more stable solid electrolyte interphase(SEI)*** as-assembled LiFePO4||Li batteries deliver a high specific capacity of 159 mA h g-1 with the capacity retention of 95.5%after 200 cycles at 30℃,as well as superior rate performance and cycling stability compared to that using the blank SPE.

关键词： Vermiculite nanosheets Two-dimensional silica Solid polymer electrolytes FillersLithium metal batteries

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On Penalized Goal-Reaching Probability Minimization with a Common Shock for an AAI

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Journal of Systems Science & Complexity 2024年

作者： HUANG Ying HUANG ya zhou Jieming School of Mathematics and Statistics Central South University School of Business Hunan Normal University MOE-LCSM School of Mathematics and Statistics Hunan Normal University Key Laboratory of Applied Statistics and Data Science Hunan Normal University College of Hunan Provinc

The authors consider a robust optimal reinsurance and investment problem in a risk model with two dependent classes of insurance business for an Ambiguity-Averse insurer(AAI). The insurer aims to minimize the goal-reaching probability that the value of the wealth process reaches a low barrier before a high goal. Using the stochastic control approach based on the Hamilton-JacobiBellman(HJB) equation, the authors derive the robust optimal reinsurance and investment strategies,as well as the corresponding value function. The authors conclude that the robust optimal investmentreinsurance strategy coincides with the one without model ambiguity, but the value function differs. As a consequence, ignoring model uncertainty leads to significant value function loss for the AAI. Besides,it is worth noting that if the insurer has only one business, the sum of the degenerated value function and the one of(Luo, et al., 2019) is equal to 1 both for ambiguity and ambiguity-neutral. Finally,numerical examples are given to illustrate our results.

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Development of Ti–V–Cr–Mn–Mo–Ce high-entropy alloys for high-density hydrogen storage in water bath environments

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Rare Metals 2024年第10期43卷 5229-5241页

作者： Hua-zhou Hu Hou-Qun Xiao Xin-Cong He Wen-Hao zhou Xiao-Xuan Zhang Rui-Zhu Tang Jie Li chuan-Ming Ma Qing-Jun Chen Key Laboratory of Rare Earths Chinese Academy of SciencesJiangxi Institute of Rare EarthsGanjiang Innovation AcademyChinese Academy of Sciences

The V-based body-centered cubic （BCC）-type hydrogen storage alloys have attracted significant attention due to their high theoretical hydrogen storage capacity of3.80 wt%.However,their practical application faces challenges related to low dehydriding capacity and poor activation *** overcome these challenges,a BCC-type Ti–V–Cr–Mn–Mo–Ce high-entropy alloy（HEA） with an effectively dehydriding capacity of 2.5 wt% above 0.1 MPa was *** introduction of Mo and conducting heat treatment,the precipitation of Ti-rich phase in HEA was successfully suppressed,resulting in improved compositional uniformity and dehydriding ***,the effective dehydriding capacity increased significantly from 0.60 wt% to 2.50 wt% a65℃,surpassing that of other types of hydrogen storage alloys under the same ***,the addition of 1 wt%Ce enabled initial hydrogen absorption at 25℃ without the need for activation at 400℃.Furthermore,Ce doping reduced the dehydriding activation energy of the Ti–V–Cr–Mn–Mo–Ce HEA from 52.71 to 42.82 kJ·mol-1Additionally,the enthalpy value of dehydrogenation decreased from 46.89 to 17.96 k J·mol-1,attributed to a decrease in the hysteresis factor from 0.68 to *** findings provide valuable insights for optimizing the hydrogen storage property of HEA.

关键词： BCC structure Ce doping Heat treatment High-entropy alloys Hydrogen storage alloys

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Plutonium utilization in a small modular molten-salt reactor based on a batch fuel reprocessing scheme

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Nuclear Science and Techniques 2024年第4期35卷 15-28页

作者： Xue-Chao Zhao Rui yan Gui-Feng Zhu ya-Fen Liu Jian Guo Xiang-zhou Cai yang Zou Shanghai Institute of Applied Physics Chinese Academy of SciencesShanghai 201800China CAS Innovative Academies in TMSR Energy System Chinese Academy of SciencesShanghai 201800China University of Chinese Academy of Sciences Beijing 100049China

A molten salt reactor(MSR)has outstanding features considering the application of thorium fuel,inherent safety,sustainability,and resistance to ***,fissile material^(233)U is significantly rare at the current stage,thus it is difficult for MSR to achieve a pure thorium-uranium fuel ***,using plutonium or enriched uranium as the initial fuel for MSR is more *** this study,we aim to verify the feasibility of a small modular MSR that utilizes plutonium as the starting fuel(SM-MSR-Pu),and highlight its advantages and ***,the structural design and fuel management scheme of the SM-MSR-Pu were ***,the neutronic characteristics,such as the graphite-irradiation lifetime,burn-up performance,and coefficient of temperature reactivity were calculated to analyze the physical characteristics of the *** results indicate that plutonium is a feasible and advantageous starting fuel for a SM-MSR;however,there are certain shortcomings that need to be *** a 250 MWth SM-MSR-Pu,approximately 288.64 kg^(233)U of plutonium with a purity of greater than 90% is produced while 978.00 kg is burned every ten *** temperature reactivity coefficient decreases from -4.0 to -6.5 pcm K^(-1) over the 50-year operating time,which ensures a long-term safe ***,the amount of plutonium and accumulation of minor actinides(MAs)would increase as the burn-up time increases,and the annual production and purity of^(233)U will *** achieve an optimal burn-up performance,setting the entire operation time to 30 years is ***,more than 3600 kg of plutonium eventually accumulate in the *** research is required to effectively utilize this accumulated plutonium.

关键词： Molten salt fuel Plutonium utilization ^(233)U TRUs mole fraction Temperature feedback coefficient

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Copper-based electro-catalytic nitrate reduction to ammonia from water:Mechanism,preparation,and research directions

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Environmental Science and Ecotechnology 2024年第4期20卷 42-62页

作者： Jinshan Wei Yi Li Hexing Lin Xihui Lu Chucheng zhou ya-yun Li Shenzhen Key Laboratory of Special Functional Materials&Shenzhen Engineering Laboratory for Advance Technology of Ceramics College of Materials Science and EngineeringShenzhen UniversityShenzhen518060PR China

Global water bodies are increasingly imperiled by nitrate pollution,primarily originating from industrial waste,agricultural runoffs,and urban *** escalating environmental crisis challenges traditional water treatment paradigms and necessitates innovative ***-catalysis,especially utilizing copper-based catalysts,known for their efficiency,cost-effectiveness,and eco-friendliness,offer a promising avenue for the electro-catalytic reduction of nitrate to *** this review,we systematically consolidate current research on diverse copper-based catalysts,including pure Cu,Cu alloys,oxides,single-atom entities,and ***,we assess their catalytic performance,operational mechanisms,and future research directions to find effective,long-term solutions to water purification and ammonia ***-catalysis technology shows the potential in mitigating nitrate pollution and has strategic importance in sustainable environmental *** to the application,challenges regarding complexity of the real water,the scale-up of the commerical catalysts,and the efficient collection of produced NH3 are still *** reseraches of catalyst specially on long term stability and in situ mechanisms are proposed.

关键词： Water treatment Nitrate removal Electrocatalysis Cu catalysts Ammonia synthesis

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Enhanced Crystallization of Poly(butylene adipate-co-terephthalate)by a Self-assembly Nucleating Agent

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Chinese Journal of Polymer Science 2024年第5期42卷 663-674,I0010页

作者： Cheng zhou Kun Chen Zi-Heng Zhang Meng-Fan Jing Chun-Tai Liu Chang-Yu Shen ya-Ming Wang State Key Laboratory of Structural Analysis Optimization and CAE Software for Industrial EquipmentNational Engineering Research Center for Advanced Polymer Processing TechnologyZhengzhou UniversityZhengzhou450002China

Poly(butylene adipate-co-terephthalate)(PBAT)is a promising biodegradable flexible polymer but suffers from slow crystallization rate,making it less attractive for some applications like the injection-molded products in comparison with low-density polyethylene(LDPE).This work aimed to accelerate the crystallization of PBAT by adding a self-assembly nucleating agent octamethylenedicarboxylic dibenzoylhydrazide(OMBH).PBAT/OMBH composites with various OMBH contents(0 wt%,0.5 wt%,0.7 wt%,1 wt%,2 wt%,3 wt%and 5 wt%)were prepared through *** effect of OMBH on the crystallization behavior,morphologies and mechanical properties of PBAT was *** highest nucleation efficiency value of 59.6%was achieved for PBAT with 0.7 wt%OMBH,much higher than that of 22.7%for PBAT with 0.7 wt%*** force microscopy results showed that OMBH formed fine fibers and induced the formation of transcrystalline layers of *** transform infrared spectroscopy(FTIR)combined with two-dimensional correlation spectra suggested that the intermolecular dipole-dipole N—H…O=C interactions but not hydrogen bond between OMBH and PBAT promoted the crystallization of PBAT in the initial period of *** presence of OMBH did not change the crystal form of PBAT but had positive contribution in enhancing its crystallinity and mechanical *** work is essential for preparing PBAT with high crystallization rate,enhancing its potential applications in injection-molded products.

关键词： Poly(butylene adipate-co-terephthalate) Biodegradable Self-assembly nucleating agent Crystallization

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