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Efficient ammonia production over e_(g)-occupancy-optimized perovskite electrocatalysts

Nano Research 2024年第6期17卷 4682-4686页

作者： Mingfa Chen Yu zhang Fulong Liu Zhenbao zhang Yuming dong Yongfa Zhu Heqing Jiang Jiawei Zhu Key Laboratory of Synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi 214122China Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of SciencesQingdao 266101China School of Chemistry and Chemical Engineering Linyi UniversityLinyi 276005China Department of Chemistry Tsinghua UniversityBeijing 100084China

Renewable-energy-driven nitrate(NO_(3)^(−))electroreduction to ammonia(NH_(3))(NERA)has been an attractive technology for decarbonizing NH_(3)production and wastewater *** NERA efficiency requires electrocatalysts that are earth-abundant and show fantastic *** we report a semiempirical activity descriptor of eg occupancy(of surface B-site cations)for identifying inexpensive perovskite oxides with extremely high efficacy toward *** establish the descriptor by systematic investigations of more than 10 perovskite *** investigations demonstrate that their intrinsic NERA activities display a volcano-shaped dependence on eg occupancy and the optimized intrinsic activities are accessible at near-1 eg *** could plausibly be attributed to the favorable overlaps between surface adsorbates and vertically-oriented eg *** importantly,utilizing this descriptor,we predict a highly active,selective,and durable NERA electrocatalyst with a composition of Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3−δ)(BSCF).Because of its close-to-1 e_(g)occupancy(i.e.~1.2),the BSCF features a superior NH_(3)production rate of 0.12 g·h^(−1)·mg_(cat.)^(−1)(Faradaic efficiency of 97.8%)that is at top of the volcano plot,and substantially outperforms most NERA electrocatalysts reported in literature.

关键词： perovskite oxide nitrate electroreduction ammonia electrosynthesis eg occupancy

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MOF-derived Cu embedded into N-doped mesoporous carbon as a robust support of PdAu nanocatalysts for ethanol electrooxidation

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Rare Metals 2024年第3期43卷 1083-1094页

作者： Yu-Fu Huang Peng Wu Jun-Ping Tang Jian Yang Jing Li Shuai Chen Xue-Ling Zhao ChengChen Bin-Wei zhang Yan-yun Ma Wei-Heng Shi dong-Hai Lin Shi-Gang Sun School of Energy and Materials Shanghai Engineering Research Center of Advanced Thermal Functional MaterialsShanghai Key Laboratory of Engineering Materials Application and EvaluationShanghai Polytechnic UniversityShanghai201209China State Key Laboratory of Physical Chemistry of Solid Surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China School of Chemistry and Chemical Engineering Chongqing UniversityChongqing401331China Center of Advanced Energy Technology and Electrochemistry Institute of Advanced Interdisciplinary StudiesChongqing UniversityChongqing400044China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou215123China Department of Materials Science and Engineering Drexel UniversityPhiladelphiaPA19104USA

Metal-organic frameworks(MOFs)h ave attracted widespread attention due to their large surface area and porous *** designing the nanostructures of MOFs to promote their application in ethanol electrooxidation is still a ***,a novel Cu-NCNs(Cu-nitrogen-doped carbon nanotubes)support was synthesized by pyrolysis of melamine(MEL)and Cu-ZIF-8 together,and then,Pd-Au nanoalloys were loaded by sodium borohydride reduction method to prepare PdAu@Cu-NCNs *** generating mesoporous carbon with high specific surface area and favorable electron and mass transport can be used as a potential excellent carrier for PdAu *** addition,the balance of catalyst composition and surface structure was tuned by controlling the content of Pd and ***,the best-performed Pd_(2)Au_(2)@Cu-NCN-1000-2(where 1000 means the carrier calcination temperature,and 2 means the calcination constant temperature time)catalyst exhibits better long-term stability and electrochemical activity for ethanol oxidation in alkaline media(4.80 A·mg^(-1)),which is 5.05 times higher than that of commercial Pd/C(0.95 A·mg^(-1)).Therefore,this work is beneficial to further promoting the application of MOFs in direct ethanol fuel cells(DEFCs)and can be used as inspiration for the design of more efficient catalyst support structures.

关键词： Metal-organic frameworks(MOFs) N-doped Mesoporous carbon PdAu Ethanol electrooxidation

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Enhanced Sampling Simulations on Transition-Metal-Catalyzed Organic Reactions:Zirconocene-Catalyzed Propylene Polymerization and Sharpless Epoxidation

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CCS Chemistry 2024年第4期6卷 964-975页

作者： Xu Han Tian-Yu Sun Yi Isaac Yang Jun zhang Jing Qiu Zhaoping Xiong Nan Qiao yun-dong Wu Yi Qin Gao Institute of Theoretical and Computational Chemistry College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871 Shenzhen Bay Laboratory Shenzhen 518132 Changping Laboratory Beijing 102200 Laboratory of Health Intelligence Huawei Cloud Computing Technologies Co.Ltd.Guizhou 550025

The bond breaking and forming in chemical reactions is a typical rare event,which is one of the difficult problems in molecular dynamics *** enhanced sampling methods have been developed to extend the time scale covered by molecular ***,the difficulties of obtaining appropriate collective variables from complicated reaction pathways and a controlled sampling over the desired phase space remain as ***,we use MetaITS,which combines metadynamics and integrated tempered sampling,to increase the sampling efficiency for chemical *** with collective variables obtained by harmonic linear discriminant analysis can efficiently decrease the main energy barrier of chemical ***,integrated tempered sampling can enhance the exploration of other degrees of *** this study,we applied the MetaITS method to two transition-metal-catalyzed organic reactions with complicated reaction *** simulated here a zirconocene-catalyzed propylene polymerization to investigate the regioselectivity and temperature *** also studied a Sharpless epoxidation reaction,for which both chiral products are observed through simulation.

关键词： molecular dynamics enhanced sampling metadynamics integrated tempering sampling propylene polymerization Sharpless epoxidation

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Visibility restoration for real-world hazy images via improved physical model and Gaussian total variation

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Frontiers of Computer Science 2024年第1期18卷 267-269页

作者： Chuan LI Enping HU Xinyu zhang Hao ZHOU Hailing XIONG yun LIU College of Computer and Information Science Southwest UniversityChongqing 400715China School of Big Data and Intelligent Engineering Chongqing College of International Business and EconomicsChongqing 401520China College of Artificial Intelligence Southwest UniversityChongqing 400715China College of Electronic and Information Engineering Southwest UniversityChongqing 400715China

1 Introduction Under real-world haze conditions,the existence of haze particles in the atmosphere reduces the visibility of captured ***,the noise is inevitably introduced into the degraded image,which further deteriorates the visual quality of the *** enhance the visibility and quality of outdoor real-world hazy images,numerous algorithms have been proposed to remove haze from a single input *** existing methods are broadly lumped into two categories:prior-based methods[1,2]and learning-based methods[3–6].Unfortunately,the widely used atmospheric scattering model and the corresponding haze removal methods fail to take the noise interference into account,which may result in poor visibility restoration performance.

关键词： visibility remove noise

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D-band center coordination modulated enzyme-like activity in Fe-Cu dual-metal single-atom nanozymes

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Nano Research 2024年第7期17卷 5872-5883页

作者： Ling Liu Shaofang zhang Guo Li Yadong Zhe Jiamin Liu Xinxu zhang Jiahao Wei Xin Sun Yonghui Li Xiao-dong zhang Tianjin Key Laboratory of Brain Science and Neural Engineering Academy of Medical Engineering and Translational MedicineTianjin UniversityTianjin 300072China Department of Physics and Tianjin Key Laboratory of Low Dimensional Materials Physics and Preparing Technology School of SciencesTianjin UniversityTianjin 300350China

After explorations in a diversity of single-atom nanozymes(SAzymes),developing dual-centered SAzymes becomes a promising approach for superior catalytic *** confusing mechanisms including atomic coordination,spatial configuration,and metal–metal atom interaction hinder the development and design of ***,a dual-centered Fe-Cu-N_(x)SAzyme exhibits excellent peroxidase(POD)-and catalase(CAT)-like activities with d-band center(ε_(d))coordination of Fe and Cu in multiple reaction stages,which plays a critical role in the adsorption of H_(2)O_(2)molecule and H_(2)O and O_(2)***,the dband center coordination,which can be represented byε_(d)(Fe)–ε_(d)(Cu)shifts,leads to the competition between one-side and bilateral adsorption,which determines the favorable reaction path with lower energy *** on experimental statistics,simulated formation energies,and reaction barriers,3 configurations,Fe-Cu-N6-I,Fe-Cu-N_(8)-II,and Fe-Cu-N_(8)-III,are modeled and ***,configuration-dependent catalytic selectivity and the competition between one-side and bilateral adsorption can be unveiled by d-band center coordination paradigm *** simulations suggest that the unsymmetrical charge distribution over the three Fe-Cu configurations could tune the adsorption strength compared with the counterparts FeN_(4)and CuN_(4).The present work provides a potential route for optimizing enzyme-like catalysis by designing the dual-or even triple-metal SAzymes,which demonstrates the large space to modulate the metal atomic configuration and interaction.

关键词： single-atom catalysis Fe-Cu dual-metal d-band center coordination enzyme mimicking competitive adsorption mechanisms

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Therapeutic effect of manual massage on early postpartum rectus abdominis separation and postpartum depression

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World Journal of Psychiatry 2024年第5期14卷 678-685页

作者： yun Chen Xiao-Yan Sun Cheng Qian Xiao-Xing zhang Yin-Jian Zhou Hong-yun zhang Zhen-Wei Xie Department of Gynecology Women’s Hospital School of Medicine Zhejiang UniversityHangzhou 310006Zhejiang ProvinceChina Department of Obstetrics and Gynecology Huzhou Maternity and Child Health Care HospitalHuzhou 313000Zhejiang ProvinceChina Department of Surgery Huzhou Maternity and Child Health Care HospitalHuzhou 313000Zhejiang ProvinceChina Department of Obstetrics Huzhou Maternity and Child Health Care HospitalHuzhou 313000Zhejiang ProvinceChina Department of Ultrasound Women’s Hospital School of Medicine Zhejiang UniversityHangzhou 310006Zhejiang ProvinceChina

BACKGROUND Rectus abdominis separation(DRA)affects pelvic stability and body *** studies have explored the effects of manual massage on early postpartum DRA and postpartum *** To analyze the curative effect of massage on early postpartum DRA and its impact on postpartum depression and thus its ability promote the overall psychosomatic rehabilitation of postpartum *** Data were retrospectively collected on 70 primiparous women with postpartum DRA who underwent rehabilitation at the Postpartum Rehabilitation Center of Huzhou Maternal and Child Health Hospital from October 2022 to September *** patients were divided into the Group S(35 cases,biomimetic electrical stimulation treatment)and Group L(35 cases,biomimetic electrical stimulation combined with manual massage treatment).Baseline data,the edinburgh postpartum depression scale(EPDS)score,and the visual analog scale(VAS)scores for rectus abdominis distance,waist circumference,and lower back pain before and after treatment were *** No significant differences were found in the baseline data,rectus abdominis distance,waist circumference,and VAS and EPDS scores between the two groups before treatment(P>0.05).After treatment,the distance between rectus abdominis and waist circumference in Group L were significantly smaller than those in Group S(P<0.05).Furthermore,lower back pain(VAS score)and the EPDS score in Group L were significantly lower than those in Group S(P<0.05).CONCLUSION Manual massage can significantly reduce early postpartum DRA,waist circumference,and back pain and improve the patient’s mental state and postpartum depression.

关键词： Manual massage Postpartum Rectus abdominis muscle separation Postpartum depression

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基于双分支时空步态特征融合的深度学习步态识别

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控制与决策 2024年第4期39卷 1403-1408页

作者：张云佐董旭石家庄铁道大学信息科学与技术学院石家庄050043

针对现有步态识别方法易受拍摄视角、着装变化影响的问题,提出一种融合二维无肩姿态拓扑能量图(shoulderless pose topological energy maps,SPTEM)和三维局部骨骼步态特征(local skeleton gait features,LSGF)的深度学习步态识别方法.... 详细信息

针对现有步态识别方法易受拍摄视角、着装变化影响的问题,提出一种融合二维无肩姿态拓扑能量图(shoulderless pose topological energy maps,SPTEM)和三维局部骨骼步态特征(local skeleton gait features,LSGF)的深度学习步态识别方法.首先,利用轻量级BlazePose姿态估计算法提取步态视频序列中的人体姿态拓扑图以生成SPTEM,在提高检测速度的同时减弱衣物变化带来的影响;然后,引入LSGF以弥补单一能量图特征在多变视角情况下识别准确率较低的不足;最后,提出结合注意力机制的时空特征提取网络模型,并在全连接层将双流特征进行一致融合.在CASIA-B数据集上对所提出方法进行验证,并与当前主流的步态识别方法进行比较,结果表明,所提出方法在跨视角和穿大衣/棉衣条件下的步态识别率都有明显提升.

关键词：无肩姿态拓扑能量图局部骨骼步态特征 BlazePose 双流网络深度学习步态识别

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A multi-parameter-induced activation of gas therapeutic platform to remarkably amplify photodynamic therapy efficacy

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Science China Chemistry 2024年第7期67卷 2403-2411页

作者： Jie Sun Ziwen zhang Hongyu Wu Xuemei dong Chengjun dong Lixin Sun Zhiqian Guo Yingchao Liu Xianfeng Gu Chunchang Zhao Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center Institute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China Department of Medicinal Chemistry School of PharmacyFudan UniversityShanghai 201203China Shandong Provincial Hospital Affiliated to Shandong First Medical University Shandong First Medical University&Shandong Academy of Medical ScienceJinan 250021China

Gas therapy(GT)combined with photodynamic therapy(PDT)is an effective strategy to compensate for the PDT limitation caused by the hypoxic tumor microenvironment,which can greatly improve PDT *** uncontrolled leakage of gas molecules during delivery seriously hinders its practical biological ***,we report a multifunction nanomedicine that enables precise gas therapy(including carbon monoxide(CO)release and H_(2)S depletion)using a multi-parameter-induced activation gas release strategy,enlarging the PDT *** nanomedicine uses a disulfide bond to covalently link a photosensitizer with the CO donor 3-hydroxyflavone(3-HF).The disulfide bond can be specifically consumed in H_(2)S-rich tumor areas,releasing the CO donor(3-HF),and also depleting H_(2)*** importantly,the photo-controlled production of^(1)O_(2)can induce 3-HF precise release of CO in the tumor *** H_(2)S,light,and^(1)O_(2)multi-parameter-induced activation of gas release strategy ensures the accuracy of GT to amplify PDT *** expected,in vitro and in vivo investigations show that GT makes up for the PDT limitation,exhibiting the highest tumor therapeutic *** multi-parameter-activated design strategy provides a new way to improve the precision and efficacy of multimodal synergistic therapy of tumors.

关键词： gas therapy precision gas release hydrogen sulfide depletion photodynamic therapy multimodal synergistic therapy

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Bacterial communities and enzyme activities during litter decomposition of Elymus nutans leaf on the Qinghai-Tibet Plateau

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Journal of Mountain Science 2024年第10期21卷 3249-3262页

作者： zhang Zhiyang JIAO Yi dong Xiaogang MA Yinshan zhang Shiting State Key Laboratory of Herbage Improvement and Grassland Agro-ecosystems College of EcologyLanzhou UniversityLanzhou 730000China Center for Volatile Interactions(VOLT)and Terrestrial Ecology Section Department of BiologyUniversity of CopenhagenCopenhagen DK-2100Denmark College of Agriculture and Ecological Engineering Hexi UniversityZhangye 734000China

The dominant plant litter plays a crucial role in carbon(C)and nutrients cycling as well as ecosystem functions maintenance on the Qinghai-Tibet Plateau(QTP).The impact of litter decomposition of dominant plants on edaphic parameters and grassland productivity has been extensively studied,while its decomposition processes and relevant mechanisms in this area remain poorly *** conducted a three-year litter decomposition experiment in the Gansu Gannan Grassland Ecosystem National Observation and Research Station,an alpine meadow ecosystem on the QTP,to investigate changes in litter enzyme activities and bacterial and fungal communities,and clarify how these critical factors regulated the decomposition of dominant plant Elymus nutans(***)*** results showed that cellulose and hemicellulose,which accounted for 95%of the initial lignocellulose content,were the main components in *** litter *** litter enzyme activities ofβ-1,4-glucosidase(BG),β-1,4-xylosidase(BX),andβ-D-cellobiosidase(CBH)decreased with decomposition while acid phosphatase,leucine aminopeptidase,and phenol oxidase increased with *** found that both litter bacterial and fungal communities changed significantly with ***,bacterial communities shifted from copiotrophic-dominated to oligotrophic-dominated in the late stage of litter *** least squares path model revealed that the decomposition of *** litter was mainly driven by bacterial communities and their secreted *** and Proteobacteria were important producers of enzymes BG,BX,and CBH,and their relative abundances were tightly positively related to the content of cellulose and hemicellulose,indicating that Bacteroidota and Proteobacteria are the main bacterial taxa of the decomposition of *** *** conclusion,this study demonstrates that bacterial communities are the main driving forces behind the decomposition of *** litter,high

关键词： Litter decomposition Lignocellulose matrix Bacterial community Litter enzyme activity Elymus nutans Qinghai-Tibet Plateau

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NaBH4-induced phase transition of CoSe_(2) with abundant Se deficiency for acidic oxygen reduction to hydrogen peroxide

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Rare Metals 2024年第2期43卷 500-510页

作者： Cai-Di Han Yong-Chao zhang Qian zhang Jin-Ting Wu Jian Gao Ji-Jun Zou Xiao-dong Zhu State Key Laboratory Base of Eco-Chemical Engineering College of Chemical Engineering Qingdao University of Science and TechnologyQingdao266042China Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China

Electrocatalytic oxygen reduction(ORR)via the 2e−pathway to form H_(2)O_(2) in acidic medium has attracted extensive ***,the low activity,insufficient selectivity and high cost of catalysts have been the ***,CoSe_(2) with abundant Se deficiency was synthesized by a simple hydrothermal method,and the addition of NaBH4-induced CoSe_(2) phase transition from orthorhombic to cubic phase with more Se *** cubic phase CoSe_(2) with abundant Se deficiency can effectively regulate the surface electronic structure with suitable binding energies of*OOH and*O,which shows high activity,selectivity and long-term stability for acidic ORR to H_(2)O_(2).The onset potential is as low as 0.73 V *** hydrogen electrode(RHE),the H_(2)O_(2) selectivity is 84%(0 V ***),and the average electron transfer number is about ***,the H_(2)O_(2) yield measured using a flow cell is as high as 115.92 mmol·gcat.^(−1)·h^(−1) and the Faradaic efficiency is 70%at 0 V ***,which presents high potential in electrocatalytic acidic ORR to H_(2)O_(2) and organic pollutant degradation using the electron-Fenton process.

关键词： Se defected CoSe_(2) Crystal phase transition Electrocatalysis Acidic oxygen reduction Hydrogen peroxide

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