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Journal of magnesium and Alloys 2024年第6期12卷 2360-2379页

作者： D.v.mashtalyar I.M.Imshinetskiy v.v.Kashepa K.v.Nadaraia M.A.Piatkova A.I.Pleshkova K.A.Fomenko A.Yu.Ustinov S.l.Sinebryukhov S.v.Gnedenkov Institute of Chemistry Far Eastern BranchRussian Academy of SciencesVladivostok690022Russia Far Eastern Federal University Vladivostok690950Russia Regional Clinical Dermatovenerological Dispensary Vladivostok690033Russia

The present study investigates the physical and chemical characteristics,behavior in vitro and in vivo,and biocompatibility of coatings containing ta_(2)O_(5),which are obtained by plasma electrolytic oxidation(PEO)on ma8 magnesium *** obtained coatings demonstrate in vivo biocompatibility and in vitro *** to the base PEO coating,the layers containing ta_(2)O_(5)facilitate the development of apatite in simulated body fluid,suggesting that the inclusion of nanoparticles improves bioactivity of the *** was found that incorporation of ta_(2)O_(5)nanoparticles increases roughness and porosity of the formed layers by increasing particle concentration in electrolytes for the PEO process contributing to sufficient soft tissue ingrowth in *** on in vivo studies,these coatings also provide favorable tissue response and minimal inflammatory reaction in comparison with the bare magnesium alloy due to protection of living tissues from deleterious corrosion events of magnesium implant such as local alkalization and intense hydrogen *** results obtained in the present study concluded biocompatibility,tissue integration of the PEO coatings containing ta_(2)O_(5)nanoparticles making them a promising protective layer for biodegradable magnesium implants.

关键词： Plasma electrolytic oxidation Bioactive coatings tantalum pentoxide Simulated body fluid(SBF) Apatite formation Histology

Polyacrylate modiﬁed Cu electrode for selective electrochemical CO_(2) reduction towards multicarbon products

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Science Bulletin 2024年第15期69卷 2395-2404页

作者： Yuchuan Shi Kaini Zhang Chung-li Dong ta Thi Thuy Nga Miao Wang Daixing Wei Jialin Wang Yiqing Wang Shaohua Shen International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power EngineeringXi’an Jiaotong UniversityXi’an 710049China Department of Physics Tamkang UniversityNew Taipei City 25137China

Highly selective production of value-added multicarbon(C^(2+))products via electrochemical CO_(2) reduction reaction(eCO_(2)RR)on polycrystalline copper(Cu)remains ***,the facile surface modification using poly(α-ethyl cyanoacrylate)(PECA)is presented to greatly enhance the C^(2+)selectivity for eCO_(2)RR over polycrystalline Cu,with Faradaic efficiency(FE)towards C^(2+)products increased from30.1%for the Cu electrode to 72.6%for the obtained Cu-PECA electrode at-1.1 v *** hydrogen electrode(RHE).Given the well-determined FEs towards C^(2+)products,the partial current densities for C^(2+)production could be estimated to be-145.4 ma cm~(-2)for the Cu-PECA electrode at-0.9 v *** in a homemade flow ***-situ spectral characterizations and theoretical calculations reveal that PECA featured with electron-accepting-C≡N and-COOR groups decorated onto the Cu electrode could inhibit the adsorption of^(*)H intermediates and stabilize the^(*)CO intermediates,given the redistributed interfacial electron density and the raised energy level of d-band center(E_(d))of Cu active sites,thus facilitating the C-C coupling and then the C^(2+)selective *** study is believed to be guidable to the modification of electrocatalysts and electrodes with polymers to steer the surface adsorption behaviors of reaction intermediates to realize practical eCO_(2)RR towards value-added C^(2+)products with high activity and selectivity.

关键词： Electrochemical CO_(2)reduction Polymer modification Electron transfer C_(2+)products

Polysulfide regulation by defect-modulated ta_(3)N_(5-x) electrocatalyst toward superior room-temperature sodium-sulfur batteries

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Science Bulletin 2024年第2期69卷 197-208页

作者： Zhen Zhang Dan luo Jun Chen Chuyin ma matthew li Haoze Zhang Renfei Feng Rui Gao Haozhen Dou Aiping Yu Xin Wang Zhongwei Chen Department of Chemical Engineering Waterloo Institute for NanotechnologyUniversity of WaterlooWaterloo N2L 3G1Canada Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023China South China Academy of Advanced Optoelectronics&International Academy of Optoelectronics at Zhaoqing South China Normal UniversityGuangzhou 510006China Chemical Sciences and Engineering Division Argonne National LaboratoryLemont 60439USA Canadian light Source Saskatoon S7N 2V3Canada

Resolving low sulfur reaction activity and severe polysulfide dissolution remains challenging in metalsulfur *** by a theoretical prediction,herein,we strategically propose nitrogenvacancy tantalum nitride(ta3N5-x)impregnated inside the interconnected nanopores of nitrogendecorated carbon matrix as a new electrocatalyst for regulating sulfur redox reactions in roomtemperature sodium-sulfur *** a pore-constriction mechanism,the nitrogen vacancies are controllably constructed during the nucleation of *** defect manipulation on the local environment enables well-regulated ta 5d-orbital energy level,not only modulating band structure toward enhanced intrinsic conductivity of ta-based materials,but also promoting polysulfide stabilization and achieving bifunctional catalytic capability toward completely reversible polysulfide ***,the interconnected continuous ta3N5-x-in-pore structure facilitates electron and sodium-ion transport and accommodates volume expansion of sulfur species while suppressing their shuttle *** to these attributes,the as-developed ta3N5-x-based electrode achieves superior rate capability of 730 mah g-1 at 3.35 A g-1,long-term cycling stability over 2000 cycles,and high areal capacity over 6 mah cm-2 under high sulfur loading of 6.2 mg *** work not only presents a new sulfur electrocatalyst candidate for metal-sulfur batteries,but also sheds light on the controllable material design of defect structure in hopes of inspiring new ideas and directions for future research.

关键词： tantalum nitride Nitrogen defects Sodium-sulfur batteries Electrocatalysts Polysulfide conversion

Enhancing Green Ammonia Electrosynthesis Through Tuning Sn vacancies in Sn‑Based MXene/ maX Hybrids

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Nano-Micro letters 2024年第5期16卷 154-168页

作者： Xinyu Dai Zhen‑Yi Du Ying Sun Ping Chen Xiaoguang Duan Junjun Zhang Hui li Yang Fu Baohua Jia lei Zhang Wenhui Fang Jieshan Qiu Tianyi ma Key laboratory for Green Synthesis and Preparative Chemistry of Advanced materials of liaoning Province College of ChemistryInstitute of Clean Energy ChemistryLiaoning UniversityShenyang 110036People’s Republic of China State Key laboratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan 030024People’s Republic of China School of Chemistry and Chemical Engineering Anhui UniversityHefei 230601People’s Republic of China School of Chemical Engineering The University of AdelaideAdelaideSA 5005Australia State Key laboratory of High‑Efficiency Utilization of Coal and Green Chemical Engineering College of Chemistry and Chemical EngineeringNingxia UniversityYinchuan 750021NingxiaPeople’s Republic of China School of Science RMIT UniversityMelbourneVIC 3000Australia Guangdong Provincial Key laboratory of Advanced Energy Storage materials School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640People’s Republic of China College of Chemical Engineering State Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing 100029People’s Republic of China

Renewable energy driven N_(2) electroreduction with air as nitrogen source holds great promise for realizing scalable green ammonia ***,relevant out-lab research is still in its ***,a novel Sn-based MXene/maX hybrid with abundant Sn vacancies,Sn@Ti_(2)CTX/Ti_(2)SnC–v,was synthesized by controlled etching Sn@Ti_(2)SnC maX phase and demonstrated as an efficient electrocatalyst for electrocatalytic N2 *** to the synergistic effect of MXene/maX heterostructure,the existence of Sn vacancies and the highly dispersed Sn active sites,the obtained Sn@Ti2CTX/Ti_(2)SnC–v exhibits an optimal NH_(3) yield of 28.4μg h^(−1) mg_(cat)^(−1) with an excellent FE of 15.57% at−0.4 v versus reversible hydrogen electrode in 0.1 M Na_(2)SO_(4),as well as an ultra-long ***,this catalyst represents a satisfactory NH3 yield rate of 10.53μg h^(−1) mg^(−1) in the home-made simulation device,where commercial electrochemical photovoltaic cell was employed as power source,air and ultrapure water as feed *** as-proposed strategy represents great potential toward ammonia production in terms of financial cost according to the systematic technical economic *** work is of significance for large-scale green ammonia production.

关键词： Green ammonia synthesis N2 electroreduction Renewable energy Sn MXene/maX hybrid

Kinetic modeling of high-temperature oxidation of pure Mg

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Journal of magnesium and Alloys 2020年第3期8卷 819-831页

作者： sa ma Fangzhou Xing Na ta lijun Zhang State Key laboratory of Powder Metallurgy Central South UniversityChangshaHunan 410083P.R.China max-Planck-Institut fiir Eisenforschung GmbH Max-Planck-Straβe 140237DusseldorfGermany

A variety of experimental tracer diffusivities of Mg and O in magnesium oxide available in the literature were first *** mobilities including bulk and short-circuit diffusion of Mg and O were then obtained by means of the CAlPHAD(Calculation of Phase Diagram)***,the diffusion-controlled kinetic model of oxidation in a gas-MgO-Mg environment was developed based on the moving boundary model and Fick's law,coupling with the modified thermodynamic description of MgO.A mathematical expression for parabolic rate constant kp of the oxide scale was derived for magnesia and correlated with the thermodynamic and diffusion kinetic *** evaluated kp results were in line with the experimental ***,the oxidation process of pure magnesium at 673 K was model-predicted,and the predicted evolution of the oxide thicknesses agreed very well with the experimental *** was indicated that the grain boundaries diffusion of magnesium cations predominated the high temperature oxidation process.

关键词： MgO Diffusion Oxidation Atomic mobility CAlPHAD Wagner's model

Achieving an ion-homogenizing and corrosion-resisting interface through nitro-coordination chemistry for stable zinc metal anodes

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Journal of Energy Chemistry 2024年第7期94卷 10-18页

作者： Jizhen Wang long Jiao Qiaoyun liu Wei Xin Yechen lei Tian Zhang leixin Yang Dengkun Shu Shuo Yang Kaihua li Chenyang li Chao Yi Hongyuan Bai Yuchao ma Huan li Wenjun Zhang Bowen'Cheng schoolof light Industry Science and Engineering State Key Laboratory of Biobased Fiber Manufacturing TechnologyTianjin Key Laboratory of Pulp and PaperChina Light Industry Key Laboratory of Papermaking and BiorefineryTianjin University of Science&TechnologyTianjin 300457China Department of materials Science and Engineering &Center of Super-Diamond and Advanced FilmsCity University of Hong Kong83 Tat Chee AvenueHong Kong 999077China School of Chemical Engineering and Advanced materials The University of AdelaideAdelaideSA 5005Australia

Suppression of uncontrollable dendrite growth and water-induced side reactions of Zn metal anodes is crucial for achieving long-lasting cycling stability and facilitating the practical implementations of aqueous Zn-metal *** address these challenges,we report in this study a functional nitro-cellulose interfacial layer(NCIl)on the surface of Zn anodes enlightened by a nitro-coordination chemistry *** NCIl exhibits strong zincophilicity and superior coordination capability with Zn^(2+)due to the highly electronegative and highly nucleophilic nature of the nitro functional *** characteristic facilitates a rapid Zn-ion desolvation process and homogeneous Zn plating,effectively preventing H_(2) evolution and dendrite ***,the negatively charged surface of NCIl acts as a shield,repelling SO_(4)^(2-)anions and inhibiting corrosive reactions on the Zn ***,reversible and stable Zn plating/stripping is achieved for over 5100 h at a current density of 1 ma cm^(-2),which is nearly 30 times longer than that of bare Zn ***,the Zn/v_(2)O_(5) full cells with the functional interface layer deliver a high-capacity retention of 80.3%for over 10,000 cycles at 5 A g^(-1).This research offers valuable insights for the rational development of advanced protective interface layers in order to achieve ultra-long-lifeZnmetal batteries.

关键词： Zinc metal anode Nitro-cellulose interfacial layer Coordination capability Dendrite-free deposition long-term cycling

具有非对称配位结构的硫族杂原子掺杂Ni-N-C单原子催化剂及其电化学二氧化碳还原性能（英文）

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Chinese Journal of Catalysis 2024年第9期 54-65页

作者：王佳琳张凯妮 ta Thi Thuy Nga 王亦清石玉川魏代星董崇礼沈少华西安交通大学能源与动力工程学院淡江大学物理系

电化学二氧化碳还原反应（eCO2RR）作为一种能将CO2转化为高附加值碳基燃料的清洁技术,对于实现碳中和具有重要意义.近年来,过渡金属单原子催化剂（M-N-C saCs）因具备出色的稳定性、活性以及较高的原子利用效率,已被广泛认为是用于eCO... 详细信息

电化学二氧化碳还原反应（eCO2RR）作为一种能将CO2转化为高附加值碳基燃料的清洁技术,对于实现碳中和具有重要意义.近年来,过渡金属单原子催化剂（M-N-C saCs）因具备出色的稳定性、活性以及较高的原子利用效率,已被广泛认为是用于eCO2RR生产CO中极具潜力的催化剂之一.其中,具有饱和对称配位结构的Ni-N4已被证实是eCO2RR的活性中心.然而,Ni-N4-C saCs中心金属周围对称的几何结构和电子构型导致其在eCO2RR过程中能垒较高.同时,其电催化活性也仍有待提升.为了调控M-N-C saCs中心金属周围电子排布,本文分别使用S粉、Se粉和Te粉作为杂原子源,通过高温焙烧方法将硫族元素（如:S,Se和Te）引入对称的Ni-N4-C构型中,获得具有不对称配位环境和电子结构的Ni-X-N3-C saCs（X:S,Se和Te）.球差电镜结果表明成功合成了Ni-X-N3-C单原子催化剂,同步辐射拟合结果证明了saCs中心Ni原子与三个邻近的N原子和一个杂原子（S,Se和Te）成键形成Ni-X-N3-C配位结构.此外,X射线光电子能谱结果表明,随着杂原子（S,Se和Te）的掺杂,Ni2p轨道结合能逐渐降低,说明杂原子与金属Ni成键,导致了中心金属Ni原子周围电荷分布明显变化.配位原子电负性大小顺序依次为:N>S>Se>Te,因此Ni 2p轨道的结合能大小趋势为:Ni-N4-C> Ni-S-N3-C> Ni-Se-N3-C> Ni-Te-N3-C.同步辐射结果表明,与具有标准平面4配位（Ni-N4）的酞菁镍（NiPc）相比,Ni-X-N3-C saCs（X代表S,Se和Te）中Ni的边前峰强度明显增大,归因于杂原子的引入导致中心对称结构发生变化.理论计算结果进一步揭示了杂原子的引入会改变中心金属周围的配位环境,诱导电荷重分布,使得Ni原子的d带中心位置更接近费米能级,增强了*COOH中间体在催化剂表面的吸附强度,从而提升了eCO2RR中CO产物选择性.特别是Se掺杂使得Ni原子的d带中心最接近费米能级,从而显著降低了*COOH的形成能垒,增强了eCO2RR活性.Bader电荷计算结果表明,与Ni-S和Ni-Te活性位相比,Ni-Se活性位周围具有最多的电荷,有更强的电子亲和力,有利于eCO2RR过程中电子转移.因此,Se掺杂的Ni-Se-N3-C在-0.70 v相对标准氢电极电压下实现了最高98%的CO选择性,高于Ni-S-N3-C和Ni-Te-N3-C.基于此,以Ni-Se-N3-C和Zn箔作为阴极和阳极材料组装的Zn-CO2电池实现了1.82 mW cm-2的峰值功率密度,并在2 ma cm-2电流密度下保持超过20 h的充放电稳定性.综上所述,本文通过一种简单通用的浸渍-焙烧-酸刻蚀的方法,将杂原子（如:S,Se和Te）引入具有对称配位结构的Ni-N4-C saC中,得到具有不对称配位的Ni-X-N3-C（X代表S,Se和Te） saCs用于高效的eCO2RR.本文深入揭示了杂原子掺杂对saCs中心金属原子的配位环境和电子结构的影响作用,为合理设计具有高活性和选择性的eCO2RR催化剂提供参考.

关键词：电化学二氧化碳还原硫族杂原子单原子催化剂不对称配位 CO生成

TM_(3)(TM=v,Fe,Mo,W)single-cluster catalyst confined on porous BN for electrocatalytic nitrogen reduction

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Journal of materials Science & Technology 2022年第13期108卷 46-53页

作者： Shuaishuai Gao Zuju ma Chengwei Xiao Zhitao Cui Wei Du Xueqin Sun Qiaohong li Rongjian sa Chenghua Sun School of Environmental and materials Engineering Yantai UniversityYantai 264005China School of materials Science and Engineering Anhui University of TechnologyMaanshan 243002China State Key laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Institute of Oceanography Ocean CollegeMinjiang UniversityFuzhou 350108China College of Chemical Engineering and Energy Technology Dongguan University of TechnologyDongguan 523808China Department of Chemistry and Biotechnology Faculty of ScienceEngineering&TechnologySwinburne University of TechnologyHawthornVIC 3122Australia

Confined metal clusters as sub-nanometer reactors for electrocatalytic N_(2) reduction reaction(eNRR)have received increasing attention due to the unique metal-metal interaction and higher activity than singleatom ***,the inspiration of the superior capacitance and unique microenvironment with regular surface cavities of the porous boron nitride(p-BN)nanosheets,we systematically studied the catalytic activity for NRR of transition-metal single-clusters in the triplet form(v_(3),Fe_(3),Mo_(3) and W_(3))confined in the surface cavities of the p-BN sheets by spin-polarized density functional theory(DFT)*** a two-step screening strategy,Mo_(3)@p-BN was found to have high catalytic activity and selectivity with a rather low limiting potential(-0.34 v)for the *** anchored Mo_(3) singlecluster can be stably embedded on the surface cavities of the substrate preventing the diffusion of the active Mo *** importantly,the Mo atoms in the Mo_(3) single-cluster would act as“cache”to accelerate electron transfer between active metal centers and nitrogen-containing intermediates via the intimate Mo-Mo *** cooperation of Mo atoms can also provide a large number of occupied and unoccupied d orbitals to make the"donation-backdonation"mechanism more *** work not only provides a quite promising electrocatalyst for NRR,but also brings new insights into the rational design of triple-atom NRR catalysts.

关键词： Electrocatalytic N_(2)reduction Density functional theory Single-cluster Porous boron nitride

距骨骨软骨病内踝“v”形截骨自体骨软骨移植

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中国矫形外科杂志 2024年第7期32卷 654-657,662页

作者：吕岩王爱国马富强李翔白玉河南省中医院河南郑州450053 郑州市骨科医院足踝外科河南郑州450052

[目的]探讨内踝“v”形截骨自体骨软骨移植治疗距骨软骨损伤(osteochondral lesions of the talus,OlT)的临床疗效。[方法]回顾分析2018年1月—2020年6月,采用内踝“v”形截骨联合自体同侧股骨髁非负重区骨软骨移植术治疗OlT的24例患者... 详细信息

[目的]探讨内踝“v”形截骨自体骨软骨移植治疗距骨软骨损伤(osteochondral lesions of the talus,OlT)的临床疗效。[方法]回顾分析2018年1月—2020年6月,采用内踝“v”形截骨联合自体同侧股骨髁非负重区骨软骨移植术治疗OlT的24例患者,评价临床及影像资料。[结果]所有患者均顺利完成手术,无神经、血管损伤,手术时间平均(71.4±12.0)min,术中失血量平均(39.2±11.2)ml。随访时间平均(24.2±6.6)个月,与术前相比,术后1年及末次随访时疼痛vAS评分[(6.1±0.7),(1.0±0.9),(0.9±0.6),Plysholm评分无显著变化(P>0.05)。影像方面,磁共振软骨修复组织观察(magnetic resonance observation of cartilage repair tissue,MOCART)评分[(43.3±7.0),(66.5±7.1),(69.2±6.5),PlT病灶修复良好,takaku踝关节退变分级无显著变化(P>0.05)。[结论]内踝“v”形截骨联合自体骨软骨移植治疗距骨骨软骨损伤疗效安全可靠。

关键词：距骨骨软骨损伤内踝v形截骨术自体骨软骨移植股骨髁非负重区

Paleo-Mesoarchean sedimentary record in the Dharwar Craton,India:Implications for Archean ocean oxygenation

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Geoscience Frontiers 2024年第1期15卷 126-154页

作者： G.Harshitha C.manikyamba M.santosh Cheng-Xue Yang A.Keshav Krishna v.v.Sesha sai I.Panduranga Reddy CSIR-National Geophysical Research Institute(NGRI) Uppal RoadHyderabad 500007India Department of Geology Osmania UniversityHyderabad 500007India School of Earth Science and Resources China University of GeosciencesBeijing 100083China Department of Earth Science University of AdelaideAdelaide SA5005Australia Yonsei Frontier lab Yonsei UniversitySeoul 03722Republic of Korea Geological Survey of India State UnitNagpurIndia

The early Archean oceans were marked by significant redox changes which have subsequently shaped the Earth’s *** chemical sediments of banded Iron and manganese formations provide important geochemical proxies for these historical shifts in the redox conditions and to trace the ancient sedimentation patterns and *** this study,we investigate the proto-ore of the Archean Mn-formations of the sandur,Chitradurga and Shimoga greenstone belts of Dharwar Craton of southern Peninsular India,which is geochemically characterised as quartz arenites,Mn-arenites,Fe-arenites,Mn-argillites and *** geochemical systematics suggest their deposition in shallow to deeper shelf in the Archean *** detrital zircon U-Pb systematics of Mn arenites and argillites indicate their maximum depositional age of 3230±52 ma representing the oldest onset of sedimentation during the Paleo-Mesoarchean timeframe in the Chitradurga Group of Dharwar *** detrital influx proxies suggest variations in sedimentation rates associated with the Archean transgressive-regressive cycles and fluctuating hydrodynamic conditions,together reflecting an increasing trend in the contributions of recycled sediment from sandur to Chitradurga and Shimoga greenstone *** available detrital zircon ages of the Mn arenites and argillites from these greenstone belts indicate a~600 ma prolonged period of Mn deposition for which high-T hydrothermal fluids from Archean mid-oceanic ridges supplied the *** trace element compositions of the concordant detrital zircons suggest 3.3-3.1 Ga Dharwar basement TTG/granitoid source which is corroborated by the zircon crystallization temperatures of 690-820℃.The source-normalisedα-dose rates of the detrital zircons signify greater degrees of sediment transport and multi-cycle nature which correspond to the earliest episode of crustal growth in the Indian sub-continent associated with the Mesoarchean Ur supercontinent.T

关键词： Mn-arenites-argillites Dharwar Craton Zircon U-Pb geochronology Passive margin sediments Ocean oxygenation