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Oxygen‑Coordinated Single Mn Sites for Efficient Electrocatalytic Nitrate Reduction to Ammonia

Nano-Micro Letters 2024年第1期16卷 147-159页

作者： Shengbo zhang Yuankang Zha Yixing Ye Ke Li Yue Lin Lirong Zheng Guozhong Wang Yunxia zhang huajie Yin Tongfei Shi Haimin zhang Laboratory of Materials Physics Centre for Environmental and Energy NanomaterialsAnhui Key Laboratory of Nanomaterials and NanotechnologyCAS Center for Excellence in NanoscienceInstitute of Solid State PhysicsHFIPSChinese Academy of SciencesHefei 230031People’s Republic of China University of Science and Technology of China Hefei 230026People’s Republic of China Key Laboratory of Agricultural Sensors Ministry of AgricultureSchool of Information and ComputerAnhui Agricultural UniversityHefei 230026People’s Republic of China Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026People’s Republic of China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of Sciences19B Yuquan RoadBeijing 100049People’s Republic of China

Electrocatalytic nitrate reduction reaction has attracted increasing attention due to its goal of low carbon emission and environmental protection.Here,we report an efficient NitRR catalyst composed of single Mn sites with atomically dispersed oxygen(O)coordination on bacterial cellulose-converted graphitic carbon(Mn-O-C).Evidence of the atomically dispersed Mn-(O-C_(2))_(4)moieties embedding in the exposed basal plane of carbon surface is confirmed by X-ray absorption spectroscopy.As a result,the as-synthesized Mn-O-C catalyst exhibits superior NitRR activity with an NH_(3)yield rate(RNH_(3))of 1476.9±62.6μg h^(−1)cm^(−2)at−0.7 V(vs.reversible hydrogen electrode,RHE)and a faradaic efficiency(FE)of 89.0±3.8%at−0.5 V(vs.RHE)under ambient conditions.Further,when evaluated with a practical flow cell,Mn-O-C shows a high RNH_(3)of 3706.7±552.0μg h^(−1)cm^(−2)at a current density of 100 mA cm−2,2.5 times of that in the H cell.The in situ FT-IR and Raman spectroscopic studies combined with theoretical calculations indicate that the Mn-(O-C_(2))_(4)sites not only effectively inhibit the competitive hydrogen evolution reaction,but also greatly promote the adsorption and activation of nitrate(NO_(3)^(−)),thus boosting both the FE and selectivity of NH_(3)over Mn-(O-C_(2))_(4)sites.

关键词： Atomically dispersed Oxygen coordination Nitrate reduction reaction In situ spectroscopic studies Hydrogen evolution reaction

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Preparation of a Novel Green Fluorescent Carbon Quantum Dots and Application in Fe^(3+)-Specific Detection in Biological System

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Journal of Analysis and Testing 2024年第1期8卷 40-51页

作者： Xianfen zhang Wenxian Wang Lijiao Guan huajie Chen Dai Li Lipeng zhang Saipeng Huang School of Chemical Engineering Northwest UniversityXi'an 710069China Chemical Technology Academy of Shandong Province Qingdao University of Science and TechnologyJinan250014China

Trace ferric ion(Fe^(3+))detection has attracted increasing attention as an essential and indispensable role in many physiological and pathological research.The green-emitting carbon quantum dots(Green-CQDs)were obtained through a green and facile one-step hydrothermal method for the specific recognition and trace detection of Fe^(3+)in this paper.The optimal excitation and emission wavelengths of the CQDs were 395 nm and 490 nm,respectively.The stokes shift was up to 95 nm,which can effectively reduce the background fluorescence interference.In addition,it also exhibited good water solubility,stability,and high biocompatibility.The fluorescence intensity of Green-CQDs was linearly related to the concentration of Fe^(3+)(range of 0-80μmol/L),and the detection limit was as low as 59 nmol/L.These good properties were favorable and successful for Fe^(3+)detection in tap water,human serum samples and living cells.In addition,a fluorescence visual test paper(FP@CQDs)was prepared utilizing filter paper as carrier,which can quickly identify Fe^(3+)in real time,and is suitable for the visualization analysis of Fe^(3+)in environment.As an efficient nanoprobe,the Green-CQDs held great promise and bright prospects in practical application in prevention and early clinical diagnosis of Fe^(3+)-associated diseases.

关键词： Carbon quantum dots Fluorescent Hydrothermal Fe^(3+)-specific detection Cell imaging

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Comprehensive optimization of piezoelectric coefficient and depolarization temperature in Mn-doped Bi_(0.5)Na_(0.5)TiO_(3)-Bi_(0.5)K_(0.5)TiO_(3)-BaTiO_(3)lead-free piezoceramics

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Journal of Materials Science & Technology 2024年第5期172卷 255-263页

作者： Huashan Zheng Enwei Sun huajie Luo Xiaoyu zhang Yixiao Yang Bin Yang Rui zhang Shantao zhang Wenwu Cao Condensed Matter Science and Technology Institute School of Instrumentation Science and EngineeringHarbin Institute of TechnologyHarbin150080China Advanced Innovation Center for Materials Genome Engineering University of Science and Technology BeijingBeijing100083China National Laboratory of Solid State Microstructures Department of Materials Science and EngineeringCollege of Engineering and Applied Science&Collaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing210093China Department of Mathematics and Materials Research Institute The Pennsylvania State UniversityUniversity ParkPennsylvania16802United States of America

Lead-free Bi_(_(0.5))Na_(_(0.5))TiO_(3)(BNT)piezoelectric ceramics have the advantages of large coercive fields and high Curie temperatures.But the improvement of piezoelectric coefficient(d 33)is usually accompanied by a huge sacrifice of depolarization temperature(T d).In this work,a well-balanced performance of d 33 and T d is achieved in MnO_(2)-doped 0.79(Bi_(_(0.5))Na_(_(0.5))TiO_(3))-0.14(Bi_(0.5)K_(0.5)TiO_(3))-0.07BaTiO_(3)ternary ceramics.The in-corporation of 0.25 mol%MnO_(2)enhances the d 33 by more than 40%,while T d remains almost unchanged(i.e.,d 33=181 pC/N,T d=184℃).X-ray diffraction(XRD)shows that an appropriate fraction of the small axis-ratio ferroelectric phase(pseudo-cubic,P c)coexists with the long-range ferroelectric phase(tetrag-onal,T)under this MnO_(2)doping.Piezoelectric force microscopy(PFM)has revealed a special domain configuration,namely large striped and layered macro domains embedded with small nanodomains.This study provides a distinctive avenue to design BNT-based piezoelectric ceramics with high piezoelectric performance and temperature stability.

关键词： BNT-BKT-BT ceramics Mn doping Piezoelectric Depolarization temperature Phase structure

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Biomimetic porous silicon oxycarbide ceramics with improved specific strength and efficient thermal insulation

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Journal of Materials Science & Technology 2024年第1期168卷 185-193页

作者： Zhuoqing zhang Jinghan Li Lei Cao Yu Shi huajie Yang Rui Yang Fan Xie Xing zhang Shi-changxu Innovation Center for Advanced Materials Institute of Metal ResearchChinese Academy of SciencesShenyang 110016China School of Materials Science and Engineering University of Science and Technology of ChinaHefei 230026China School of Materials Science and Engineering Shenyang Ligong UniversityShenyang 110159China Shenyang Aircraft Design and Research Institute Shenyang 110035China

Considering the challenge of aerodynamic heating,the development of high-performance insulating ce-ramic materials with lightweight and low thermal conductivity is crucially important for aerospace vehi-cles to achieve flight at high speed for a long time.In this work,macro-porous silicon oxycarbide(SiOC)ceramics with directional pores(DP-SiOC)(mean pore size of 88.1μm)were prepared using polysiloxane precursors via freeze casting and photocrosslinking,followed by pyrolysis.The DP-SiOC samples were lightweight(density∼0.135 g cm^(-3))with a porosity of 90.4%,which showed good shapability through the molding of polysiloxane precursors.The DP-SiOC samples also exhibited an ultra-low thermal con-ductivity of 0.048 W(m K)^(-1)at room temperature,which can also withstand heat treatment at 1200°C for 1 h.In addition,scaffolds with triply periodic minimal surfaces(TPMS)were fabricated using digital light processing(DLP)printing,which was further filled with polysiloxane precursors for increasing the strength of DP-SiOC.The TPMS scaffolds filled with macro-porous SiOC ceramics(TPMS-DP-SiOC)showed good integration between TPMS and macro-pore structures,which had a porosity∼75%and high specific strength of 9.73×10^(3)N m kg^(-1).The thermal conductivity of TPMS-DP-SiOC samples was 0.255 W(m K)^(-1)at room temperature.The biomimetic TPMS-DP-SiOC ceramics developed in this study are likely used for thermal protection systems.

关键词： Thermal insulation Light weight Macro-porous ceramics SiOC

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Heterointerface engineering of rhombic Rh nanosheets confined on MXene for efficient methanol oxidation

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Journal of Energy Chemistry 2024年第6期93卷 419-428,I0011页

作者： Qi zhang Quanguo Jiang Xiang Yang Chi zhang Jian zhang Lu Yang Haiyan He Guobing Ying huajie Huang College of Materials Science and Engineering Hohai UniversityNanjing 210098JiangsuChina New Energy Technology Engineering Lab of Jiangsu Province College of ScienceNanjing University of Posts&Telecommunications(NUPT)Nanjing 210023JiangsuChina School of Materials Science and Engineering Southeast UniversityNanjing 211100JiangsuChina

Although metallic rhodium(Rh)is regarded as a promising platinum-alternative anode catalyst of direct methanol fuel cell(DMFC),the conventional"particle-to-face"contact model between Rh and matrix largely limits the overall electrocatalytic performance due to their insufficient cooperative effects.Herein,we report a controllable and robust heterointerface engineering strategy for the bottom-up fabrication of rhombic Rh nanosheets in situ confined on Ti_3C_(2)T_x MXene nanolamellas(Rh NS/MXene)via a convenient stereoassembly process.This unique design concept gives the resulting 2D/2D Rh NS/MXene heterostructure intriguing textural features,including large accessible surface areas,strong"face-toface"interfacial interactions,homogeneous Rh nanosheet distribution,ameliorative electronic structure,and high electronic conductivity.As a consequence,the as-prepared Rh NS/MXene nanoarchitectures exhibit exceptional electrocatalytic methanol oxidation properties in terms of a large electrochemically active surface area of 126.2 m~2 g_(Rh)~(-1),a high mass activity of 1056.9 mA mg_(Rh)-~1,and a long service life,which significantly outperform those of conventional particle-shaped Rh catalysts supported by carbon black,carbon nanotubes,reduced graphene oxide,and MXene matrixes as well as the commercial Pt nanoparticle/carbon black and Pd nanoparticle/carbon black catalysts with the same noble metal loading amount.Density functional theory calculations further demonstrate that the direct electronic interaction at the well-contacted 2D/2D heterointerfaces effectively enhances the adsorption energy of Rh nanosheets and induces a left shift of the d-band center,thereby making the Rh NS/MXene configuration suffer less from CO poisoning.This work highlights the importance of rational heterointerface design in the construction of advanced noble metal/MXene electrocatalysts,which may provide new avenues for developing the next-generation DMFC devices.

关键词： Rhodium nanosheet Ti_(3)C_(2)T_(x)MXene Heterointerface Electrocatalyst Fuel cell

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Revealing structure correlation between ionic liquid and metal-organic framework matrix

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Magnetic Resonance Letters 2024年第2期4卷 65-72页

作者： Ligang Xu Wenda zhang Chenjie Lou Chenxu Geng Yuxiu Sun Jie Liu Yongchao Shi huajie Luo Jipeng Fu Haiyan Zheng Mingxue Tang Center for High Pressure Science and Technology Advanced Research Beijing100193China College of Materials Science and Engineering Guilin University of TechnologyGuilin541004China State Key Laboratory of Separation Membranes and Membrane Processes School of Material Science and EngineeringTiangong UniversityTianjin300387China University of Science and Technology Beijing Beijing100083China Key Laboratory of Rare Earth Optoelectronic Materials and Devices of Zhejiang Province Institute of Optoelectronic Materials and DevicesChina Jiliang UniversityHangzhou310018China

Solid-state batteries are rising rapidly in response to the fast-increasing energy demand.Metal-organic framework(MOF) loaded with ionic liquids has brought new opportunities for solid-state batteries owing to its good interfacial compatibility and high ionic conductivity. MOF-808 is selected to be filled with Li-contained ionic liquid for structure and ion dynamics investigation using nuclear magnetic resonance(NMR) and X-ray diffraction.This study finds that the introduced ionic liquid would partially soften the matrix of MOF-808 and thus yield amorphous phase. By selective isotope replacement under cycling symmetric ^(6)Li metal cell, Li^(+)ion is observed to mainly go cross ionic liquid in the open channel of matrix under potential polarization.

关键词： Nuclear magnetic resonance Solid-state batteries MOF-808 Ionic liquid Local structure

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Genomic convergence underlying high-altitude adaptation in alpine plants

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Journal of Integrative Plant Biology 2023年第7期65卷 1620-1635页

作者： Xu zhang Tianhui Kuang Wenlin Dong Zhihao Qian huajie zhang Jacob BLandis Tao Feng Lijuan Li Yanxia Sun Jinling Huang Tao Deng Hengchang Wang Hang Sun CAS Key Laboratory of Plant Germplasm Enhancement and Specialty Agriculture The Chinese Academy of SciencesWuhan Botanical GardenWuhan 430074China Center of Conservation Biology Core Botanical GardensThe Chinese Academy of SciencesWuhan 430074China Yunnan International Joint Laboratory for Biodiversity of Central Asia Key Laboratory for Plant Diversity and Biogeography of East AsiaKunming Institute of BotanyThe Chinese Academy of SciencesKunming 650201China University of Chinese Academy of Sciences Beijing 100049China School of Integrative Plant Science Section of Plant Biology and the L.H.Bailey HortoriumCornell UniversityIthacaNew York 14850USA BTI Computational Biology Center Boyce Thompson InstituteIthacaNew York 14853USA State Key Laboratory of Crop Stress Adaptation and Improvement School of Life SciencesHenan UniversityKaifeng 475004China Department of Biology East Carolina UniversityGreenvilleNorth Carolina 27858USA

Evolutionary convergence is one of the most striking examples of adaptation driven by natural selection.However, genomic evidence for convergent adaptation to extreme environments remains scarce.Here, we assembled reference genomes of two alpine plants, Saussurea obvallata(Asteraceae)and Rheum alexandrae(Polygonaceae), with 37,938 and 61,463 annotated protein-coding genes. By integrating an additional five alpine genomes,we elucidated genomic convergence underlying high-altitude adaptation in alpine plants. Our results detected convergent contractions of diseaseresistance genes in alpine genomes, which might be an energy-saving strategy for surviving in hostile environments with only a few pathogens present.We identified signatures of positive selection on a set of genes involved in reproduction and respiration(e.g., MMD1, NBS1, and HPR), and revealed signatures of molecular convergence on genes involved in self-incompatibility, cell wall modification,DNA repair and stress resistance, which may underlie adaptation to extreme cold, high ultraviolet radiation and hypoxia environments. Incorporating transcriptomic data, we further demonstrated that genes associated with cuticular wax and flavonoid biosynthetic pathways exhibit higher expression levels in leafy bracts, shedding light on the genetic mechanisms of the adaptive “greenhouse” morphology. Our integrative data provide novel insights into convergent evolution at a high-taxonomic level,aiding in a deep understanding of genetic adaptation to complex environments.

关键词： adaptation alpine plants evolutionary rates genomic convergence “greenhouse”morphology high altitude

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A Systematic Investigation of Complement and Coagulation-Related Protein in Autism Spectrum Disorder Using Multiple Reaction Monitoring Technology

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Neuroscience Bulletin 2023年第11期39卷 1623-1637页

作者： Xueshan Cao Xiaoxiao Tang Chengyun Feng Jing Lin huajie zhang Qiong Liu Qihong Zheng Hongbin Zhuang Xukun Liu Haiying Li Naseer Ullah Khan Liming She College of Life Science and Oceanography Shenzhen UniversityShenzhen518060China College of Physics and Optoelectronics Engineering Shenzhen UniversityShenzhen518060China Maternal and Child Health Hospital of Baoan Shenzhen518100China Department of Endocrinology Guiyang First People’s HospitalGuiyang550002China Shenzhen-Hong Kong Institute of Brain Science-Shenzhen Fundamental Research Institutions Shenzhen518055China Shenzhen Key Laboratory of Marine Biotechnology and Ecology Shenzhen518060China

Autism spectrum disorder(ASD)is one of the common neurodevelopmental disorders in children.Its etiology and pathogenesis are poorly understood.Previous studies have suggested potential changes in the complement and coagulation pathways in individuals with ASD.In this study,using multiple reactions monitoring proteomic technology,16 of the 33 proteins involved in this pathway were identified as differentially-expressed proteins in plasma between children with ASD and controls.Among them,CFHR3,C4BPB,C4BPA,CFH,C9,SERPIND1,C8A,F9,and F11 were found to be altered in the plasma of children with ASD for the first time.SERPIND1 expression was positively correlated with the CARS score.Using the machine learning method,we obtained a panel composed of 12 differentially-expressed proteins with diagnostic potential for ASD.We also reviewed the proteins changed in this pathway in the brain and blood of patients with ASD.The complement and coagulation pathways may be activated in the peripheral blood of children with ASD and play a key role in the pathogenesis of ASD.

关键词： pathogenesis children complement

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A novel vanadium complex VO(p-dmada)inhibits neuroinflammation induced by lipopolysaccharide

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Chinese Chemical Letters 2023年第10期34卷 209-214页

作者： Zhijun He Xiaoqian Li huajie zhang Xin Liu Shuangxue Han Anwar Abdurahman Liming Shen Xiubo Du Nan Li Xiaoda Yang Qiong Liu Shenzhen Key Laboratory of Marine Biotechnology and Ecology College of Life Sciences and OceanographyShenzhen UniversityShenzhen 518055China National R&D Center for Se-rich Agricultural Products Processing Hubei Engineering Research Center for Deep Processing of Green Se-rich Agricultural ProductsSchool of Modern Industry for Selenium Science and EngineeringWuhan Polytechnic UniversityWuhan 430023China Shenzhen Bay Laboratory Shenzhen 518055China State Key Laboratories of Natural and Biomimetic Drugs Department of Chemical BiologySchool of Pharmaceutical SciencesPeking University Health Science CenterBeijing 100191China Department of Pharmacy Shenzhen People’s Hospital(The Second Clinical Medical CollegeJinan UniversityThe First Affiliated HospitalSouthern University of Science and Technology)Shenzhen 518020China Shenzhen-Hong Kong Institute of Brain Science-Shenzhen Fundamental Research Institutions Shenzhen 518055China

Uncontrolled microglial activation is decisively involved in the neuroinflammatory pathogenesis of brain diseases. Consequently, suppression of microglial overactivation appears to be a strategy for the prevention of nerve injury. In this paper, a novel vanadium complex, vanadyl N-(p-N,Ndimethylaminophenylcarbamoylmethyl)iminodiacetate(VO(p-dmada)), was synthesized from vanadyl sulfate and N,N-dimethyl-p-phenylenediamine, which was structurally characterized by Fourier transform infrared spectrum and ESI-MS analysis. The effect of VO(p-dmada) on neuroinflammation was investigated by using the models of lipopolysaccharide(LPS)-induced BV2 microglial cells and BALB/c mice.Our data demonstrated that VO(p-dmada) significantly suppressed microglial activation by downregulating inflammatory mediators and associated proteins, and inactivating nuclear factor-κ B(NF-κ B) signaling pathway. VO(p-dmada) also upregulated peroxisome proliferator activated receptor gamma(PPARγ) by reducing transglutaminase 2 and heat shock protein 60 expression. Co-treatment with PPARγ antagonist GW9662 significantly impeded the inhibitory effect of VO(p-dmada) on LPS-induced neuroinflammation.These cumulative findings demonstrated that VO(p-dmada) is a potential new drug for the treatment of neuroinflammation-related neurodegenerative diseases.

关键词： Vanadium Vanadyl N-(p-N,Ndimethylaminophenylcarbamoylmethyl)iminodiacetate (VO(p-dmada)) Neuroinflammation Microglia Proteomics Peroxisome proliferator activated receptor gamma(PPARγ)

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采用动态相关度权重的特征选择算法

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计算机工程与应用 2024年第4期60卷 89-98页

作者：许华杰刘冠霆张品秦远卓广西大学计算机与电子信息学院南宁530004 广西大学广西多媒体通信与网络技术重点实验室南宁530004 北部湾港防城港码头有限公司广西防城港538001 广西大学土木建筑工程学院南宁530004

基于互信息的特征选择算法在考虑候选特征提供的新分类信息时,通常忽略了候选特征的加入会使得已选特征和类标签的相关性发生变化而带来额外的新增信息量,以及在计算冗余信息时采用累加求和的形式可能导致低估候选特征的冗余程度。针对... 详细信息

基于互信息的特征选择算法在考虑候选特征提供的新分类信息时,通常忽略了候选特征的加入会使得已选特征和类标签的相关性发生变化而带来额外的新增信息量,以及在计算冗余信息时采用累加求和的形式可能导致低估候选特征的冗余程度。针对以上问题,提出动态相关度权重的定义,以更全面地考虑候选特征带来的新信息量成分;提出改进冗余项的定义,采用取最大值和归一化策略,以解决传统算法存在的低估冗余问题;在此基础上提出一种采用动态相关度权重的特征选择算法(feature selection using dynamic relevance weight,FSDRW)。选取五种当前主流的基于互信息的过滤式特征选择算法进行对比实验,在来自加州大学尔湾分校UCI和亚利桑那州立大学ASU的机器学习测试数据集上的实验表明,所提出的算法在分类准确率及综合性能方面具有较好的表现。最后将所提出算法应用于广西某水库工程的微震、爆破信号识别中,算法选取出的特征用于微震信号识别可达到98.86%的分类准确率,验证了算法在实际应用中的有效性。

关键词：特征选择互信息信息熵动态相关度权重

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