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Revealing interfacial charge redistribution of homologous Ru-RuS_(2) heterostructure toward robust hydrogen oxidation reaction

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Journal of Energy Chemistry 2024年第7期94卷 332-339页

作者： Yi Liu Lianrui Cheng Shuqing Zhou Yuting Yang Chenggong Niu Tayirjan taylor Isimjan Bao Wang Xiulin Yang Guangxi Key Laboratory of Low Carbon Energy Materials School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGuilin 541004GuangxiChina State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Saudi Arabia Basic Industries Corporation(SABIC)at King Abdullah University of Science and Technology(KAUST) Thuwal 23955-6900Saudi Arabia

Precisely tailoring the surface electronic structures of electrocatalysts for optimal hydrogen binding energy and hydroxide binding energy is vital to improve the sluggish kinetics of hydrogen oxidation reac-tion(hOR).herein,we employ a partial desulfurization strategy to construct a homologous Ru-RuS_(2) heterostructure anchored on hollow mesoporous carbon nanospheres(Ru-RuS_(2)@C).The disparate work functions of the heterostructure contribute to the spontaneous formation of a unique built-in electric field,accelerating charge transfer and boosting conductivity of ***,Ru-RuS_(2)@C exhibits robust hOR electrocatalytic activity,achieving an exchange current density and mass activity as high as 3.56 mA cm^(-2) and 2.13 mAμg_(Ru)^(-1),*** those of state-of-the-art Pt/C and most contemporary Ru-based hOR ***,Ru-RuS_(2)@C can tolerate 1000 ppm of cO that lacks in Pt/*** analysis reveals that the directional electron transfer across Ru-RuS_(2) heterointerface induces local charge redistribution in interfacial region,which optimizes and balances the adsorption energies of h and Oh species,as well as lowers the energy barrier for water formation,thereby promoting thehoR performance.

关键词： heterostructure hollow spherical structure hydrogen oxidation reaction Charge redistribution Density functional calculation

Valence electronic engineering of superhydrophilic Dy-evoked Ni-MOF outperforming RuO_(2) for highly efficient electrocatalytic oxygen evolution

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Journal of Energy Chemistry 2024年第3期90卷 244-252,I0007页

作者： Zhiyang huang Miao Liao Shifan Zhang Lixia Wang Mingcheng Gao Zuyang Luo Tayirjan taylor Isimjan Bao Wang Xiulin Yang Guangxi Key Laboratory of Low Carbon Energy Materials School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGulin 541004GuangxiChina State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Saudi Arabia Basic Industries Corporation(SABIC)at King Abdullah University of Science and Technology(KAUST) Thuwal 23955-6900Saudi Arabia

Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) ***,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of *** method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation *** and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and *** resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing ***,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOh as the actual active ***,Dy@Ni-MOF shows impressive OER performance,significantly surpassing ***,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.

关键词： Dy@Ni-MOF Dy incorporation Electronic interaction Superhydrophilicity Oxygen evolution reaction

Phytic acid-derivative Co_(2)B-CoPO_x coralloidal structure with delicate boron vacancy for enhanced hydrogen generation from sodium borohydride

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Chinese Chemical Letters 2024年第4期35卷 525-531页

作者： Luyan Shi Ke Zhu Yuting Yang Qinrui Liang Qimin Peng Shuqing Zhou Tayirjan taylor Isimjan Xiulin Yang Guangxi Key Laboratory of Low Carbon Energy Materials School of Chemistry and Pharmaceutical SciencesGuangxi Normal UniversityGuilin 541004China Saudi Arabia Basic Industries Corporation(SABIC)at King Abdullah University of Science and Technology(KAUST) Thuwal 23955-6900Saudi Arabia

Application of transition metal boride(TMB) catalysts towards hydrolysis of NaBh_(4) holds great significance to help relieve the energy crisis. herein, we present a facile and versatile metal-organic framework(MOF) assisted strategy to prepare Co_(2)B-CoPO_x with massive boron vacancies by introducing phytic acid(PA) cross-linked Co complexes that are acquired from reaction of PA and ZIF-67 into cobalt boride. The PA etching effectively breaks down the structure of ZIF-67 to create more vacancies, favoring the maximal exposure of active sites and elevation of catalytic activity. Experimental results demonstrate a drastic electronic interaction between Co and the dopant phosphorous(P), thereby the robustly electronegative P induces electron redistribution around the metal species, which facilitates the dissociation of B-h bond and the adsorption of h_(2)O molecules. The vacancy-rich Co_(2)B-CoPO_x catalyst exhibits scalable performance, characterized by a high hydrogen generation rate(hGR) of 7716.7 m L min^(-1)g^(-1) and a low activation energy(Ea) of 44.9 k J/mol, rivaling state-of-the-art catalysts. This work provides valuable insights for the development of advanced catalysts through P doping and boron vacancy engineering and the design of efficient and sustainable energy conversion systems.

关键词： Co_(2)B-CoPO_x catalyst P doping Boron vacancy NaBh_(4) hydrolysis hydrogen generation

构筑富含磷空位缺陷的磷化钯催化剂实现高效和抗CO毒化的碱性氢氧化反应

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Chinese Journal of Catalysis 2024年第1期56卷 176-187页

作者：杨玉婷石路岩梁沁睿刘奕董家新 Tayirjan taylor Isimjan 王宝杨秀林广西师范大学化学与药学学院广西低碳能源材料重点实验室中国广西桂林541004 中山大学环境科学与工程学院中国广东广州510275 中国科学院过程工程研究所生化工程国家重点实验室中国北京100190 阿卜杜拉国王科技大学的沙特阿拉伯基础工业公司图瓦勒沙特阿拉伯

碱性阴离子交换膜燃料电池(AEMFCs)可以直接将氢的化学能转化为电能,被认为是新兴绿色氢经济的基石技术.但其阳极氢氧化反应(hOR)动力学缓慢,严重依赖于Pt基催化剂.由于Pt基催化剂极易被CO毒化、动力学过程复杂以及价格昂贵,极大限制了... 详细信息

碱性阴离子交换膜燃料电池(AEMFCs)可以直接将氢的化学能转化为电能,被认为是新兴绿色氢经济的基石技术.但其阳极氢氧化反应(hOR)动力学缓慢,严重依赖于Pt基催化剂.由于Pt基催化剂极易被CO毒化、动力学过程复杂以及价格昂贵,极大限制了其商业化应用.因此,亟需开发高效、稳定和抗CO毒化能力强的新型hOR催化剂.Pd具有与Pt相似的氢键结合能,并且比Pt储量丰富,有望成为实现hOR的候选催化剂.然而,Pd的本征催化活性和Pt相比仍有很大差距.近年来,磷化钯因具有功能多样性和高催化活性被广泛关注.此外,缺陷工程可以有效调控催化剂的表面结构,改善中间体的吸附强度,提高催化剂的催化活性.因此,构建富含缺陷的磷化钯催化剂有望提高其hOR的性能.然而,该方向研究较少,反应机理尚不清楚.因此,阐明空位缺陷对于提高磷化钯催化剂hOR性能的作用机制,对促进AEMFCs电催化反应具有重要意义.本文通过溶胶-凝胶法以及低温磷化策略合成了一种碗状半球结构的富含磷空位Pd3P@C(V_(p)-Pd_(3)P@C)催化剂,并用于碱性hOR.在磷化过程中,通过调整Pd前驱体和磷源比例以及煅烧温度,在碳碗状半球载体上合成具有不同晶相组成(Pd/Pd_(3)P@C,Pd_(3.20)P_(12)@C,Pd_(3)P@C,和Pd_(5)P_(2)@C)的Pd_(x)P_(y)@C催化剂.扫描电镜和透射电镜证实了催化剂为碗状半球形貌.利用电子顺磁共振波谱研究了Pd_(x)P_(y)@C催化剂的磷空位浓度,结果表明,Pd/P比例为1:3时,在350℃下煅烧得到的Vp-Pd_(3)P@C具有最高的磷空位浓度.X射线光电子能谱证实了磷空位促进了d-p轨道杂化,增强了Pd和磷之间的电子相互作用.电化学测试结果表明,Vp-Pd_(3)P@C具有最高的hOR性能,Vp-Pd_(3)P@C在50 mV的质量活性为1.66 mAμg_(Pd)^(–1),交换电流密度为3.2 mA cm^(–2),优于Pd3P(0.45 mAμg_(Pd)^(-1),1.78 mA cm^(–2))和商业Pt/C(0.3 mAμg_(Pd)^(-1),2.29 mA cm^(–2)).同时,该催化剂在50 mV的电位下能稳定运行20 h.此外,即使在CO浓度高达1000 ppm时,Vp-Pd_(3)P@C催化剂仍表现出较好的hOR活性.紫外光电子能谱证实了Vp-Pd_(3)P@C中的Pd原子呈现缺电子状态,这不利于Pd 4d轨道对CO 2π^(*)轨道的电子反馈,降低了Pd和CO的键合强度,进而减弱了Pd对CO分子的吸附,从而增强了其抗CO中毒的能力.密度泛函理论计算结果表明,相较于磷空位浓度较少的Pd_(3)P@C催化剂,富含磷空位缺陷的Vp-Pd_(3)P@C催化剂能够优化和平衡反应中间体(hads和Ohads)的吸附强度,使速率决定步骤从h_(2)O^(*)的解吸转换到h_(2)O的形成,促进了Volmer反应(hads+Ohads→h_(2)O+2^(*)sites)的进行,进而提升了催化活性.系统实验和表征结果表明,Vp-Pd_(3)P@C较好的hOR性能可归因于以下3个因素:(1)空心碗状结构大大地增加了固-液-气三相接触点,加速了hOR的传质过程;(2)磷空位产生的局部反应活性和有利的电子结构优化了hads和Ohads的吸附强度,极大地促进了Volmer步骤;(3)丰富的磷空位打破了原有的周期性晶体结构,形成了新的电子结构,有效地抑制了电子从Pd 4d轨道到CO 2π^(*)轨道的反馈,提高了Vp-Pd_(3)P@C对CO的耐受能力.综上,本文通过缺陷工程策略调控了Vp-Pd_(3)P@C中活性位点与hOR关键中间体的相互作用,明确了空位缺陷浓度与hOR活性之间的构效关系.并从碱性hOR反应机理,CO分子与金属催化剂的轨道相互作用以及结构设计三个方面总结了高效和稳定的hOR催化剂的设计原则.目前,由于界面环境的复杂性和缺乏原位技术,催化剂表面上痕量中间体的光谱信息难以获得,未来可在开发原位技术监测hOR过程中间体和催化剂的组分变化方面做出更多的努力,以促进AEMFCs的商业化应用.

关键词：氢氧化反应 CO耐受性磷空位 V_(p)-Pd_(3)P@C 碗状半球

Linking 24-h Movement Behavior Guidelines to Cognitive Difficulties,Internalizing and Externalizing Problems in Preterm Youth

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International Journal of Mental health Promotion 2024年第8期26卷 651-662页

作者： Zhihui Cheng Ailikute Aikeremu Yanping Gao Zhihao Zhang Anthony G.Delli Paoli Paolo Marcello Cunha Alyx taylor Fabian herold Liye Zou Body-Brain-Mind Laboratory School of PsychologyShenzhen UniversityShenzhen518060China Department of Kinesiology and health Rutgers UniversityNew BrunswickNJ 08901USA Metropolitan University Center of Maringá Maringá87020Brazil School of health and Rehabilitation Sciences AECC University CollegeBournemouthBH52DFUK Research Group Degenerative and Chronic Diseases MovementFaculty of Health Sciences BrandenburgUniversity of PotsdamPotsdam14476Germany

Background:Given the heightened risk of developmental challenges associated with preterm birth,it is crucial to explore interventions that may ameliorate potential adverse *** study aimed to examine whether meeting the 24-h movement behavior(24-hMB)guidelines,which include recommendations on physical activity(PA),screen time(ST),and sleep(SL),is related to indicators of cognitive difficulties,internalizing problems(e.g.,depression and anxiety),and externalizing problems(e.g.,difficulties in making friends and arguing)in a sample of preterm youth(children and adolescents born preterm).Methods:In this cross-sectional study,data from 3410 preterm youth(aged 6 to 17 years)were included for data *** logistic regression was used to investigate associations between meeting the 24-hMB guidelines and the above-mentioned health outcomes,while controlling for sociodemographic and health-related ***:The prevalence of meeting 24-hMB guidelines varied across independent and integrated components of the 24-hMB *** the ST guideline alone(ph fewer cognitive difficulties and reduced internalizing and externalizing problems(phe SL guideline alone and integrated guidelines(i.e.,SL+ST)were associated with lower odds of depression and anxiety(ph less pronounced difficulties in making friends and arguing(phMB guidelines in an isolated and integrated manner are linked to better cognitive performance and fewer internalizing and externalizing problems in preterm ***:Results suggest that advocating for the implementation of the 24-hMB guidelines may reduce cognitive challenges and behavioral issues,which is of high relevance for improving public *** longitudinal studies in preterm youth should inves

关键词： Cognitive difficulties externalizing problems internalizing problems physical activity preterm youth

冷杉-铁杉林各层盖度在冷箭竹更新恢复中的变化

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生态学杂志 2017年第9期36卷 2403-2411页

作者：周世强李忠黄金燕 Alan h.taylor 刘巅张明春周小平张和民中国大熊猫保护研究中心四川都江堰611830 Department of Geography The Pennsylvania State University

本研究的目的是通过分析不同时期林分各层植物覆盖度的变化,了解冷箭竹(Bashania faberi)的自然恢复进程以及各层植物之间的相互作用。为此,在四川卧龙国家级自然保护区的冷杉-铁杉林内设置固定样地(n=7),1984—2013年分3~4次调查了样... 详细信息

本研究的目的是通过分析不同时期林分各层植物覆盖度的变化,了解冷箭竹(Bashania faberi)的自然恢复进程以及各层植物之间的相互作用。为此,在四川卧龙国家级自然保护区的冷杉-铁杉林内设置固定样地(n=7),1984—2013年分3~4次调查了样地中各层植物的覆盖度。结果表明,更新竹林的竹子盖度逐年增加,2013年达到60%以上;残存竹林的竹子盖度变化呈单峰模式,表现出先增长、到达峰值后下降的趋势;草本植物层和地被层相似,随着竹子的更新恢复,盖度低于开花枯死期;乔木林冠层的覆盖度,虽然1984年和2013年之间的显著性检验差异明显,但两年的绝对值相差较小,大约0.60%~18.89%;样地(或斑块)间的不同变化趋势主要与其所处林分的立地条件差异有关。本文还初步尝试了不同时期竹子盖度空间分布的可视化,有利于人们更为直观地洞察竹子恢复过程中的空间动态格局。

关键词：大熊猫主食竹自然更新植物盖度卧龙自然保护区

Successional trends and processes on a glacial foreland in Southern Iceland studied by repeated species counts

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Ecological Processes 2019年第1期8卷 138-148页

作者： taylor G.Glausen Lawrence h.Tanner Jacobs School of Medicine and Biomedical Sciences State University of New York at BuffaloBuffaloNY 14203USA Department of Biological and Environmental Sciences Le Moyne CollegeSyracuseNY 13214USA

Introduction:Primary succession on glacial forelands is increasingly relevant as rapid glacial retreat is exposing growing land areas to plant *** investigated temporal trends,controls,and outcomes in floral succession on a subarctic glacial ***,we examined changes in community composition(mosses,low shrubs,forbs,trees,and graminoids)over long-term(decadal)and short-term(he underlying processes responsible for the observed successional ***:The study area was the foreland of the Skaftafellsjӧkull,located in Vatnajӧkull National Park near the south coast of *** established nine transect lines at varying distances from the ice front representing surfaces of age ranging from less than one decade to over 100 *** transect consisted of five measurement stations of 1 m2 where we measured vegetative cover(VC),species richness(SR),and species density(SD)and calculated species evenness(SE).Measurements were made initially in 2007 and repeated at the same geographic coordinates in ***:VC increased with distance from the ice front from 16%to over 90%.SR and SD increased from the youngest pioneer community through a mid-successional stage corresponding to an age of over 60 but less than 100 *** VC but declining SR,SD,and SE characterized the oldest(over 100 years)bryophyte-dominated *** turnover,which involved forbs almost exclusively,increased moderately from early through midsuccessional sites and declined on older *** of the measurements made in 2014 to those made in 2007 demonstrates increased SR at mid-successional sites while SD remained relatively ***:At a small scale,colonization is controlled by local factors such as microtopography and aspect,particularly in proximity to the *** the landscape level,changes in VC and community structure are controlled by time and nutrient *** nutrient level

关键词： Primary succession Glacial foreland Species richness Species density Bryophyte

Tectonic evolution of the early Mesozoic blueschist-bearing Qiangtang metamorphic belt,central Tibet

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Tectonic evolution of the early Mesozoic blueschist-bearing ...

可重复使用的轻重量低温推进剂贮箱设计的分析研究

中国科学院地质与地球物理研究所2003学术年会

作者： Paul Kapp Craig E.Manning T.Mark harrison Michael h.taylor Department of Geosciences University of ArizonaTucsonArizonaUSA Department of Earth and Space Sciences and Institute of Geophysics and Planetary Physics University of CaliforniaLos AngelesCahforniaUSA Institute of Advanced Studies Australian National UniversityCanberraACTAustralia Department of Earth and Space Sciences and Institute of Geophysics and Planetary Physics University of CaliforniaLos AngelesCaliforniaUSA.

A>500-km-long east-west trending metamorphic belt in the Qiangtang terrane of central Tibet consists of tectonic melange that occurs in the footwalls of Late Triassic-Early Jurassic domal low-angle normal *** melange is comprised of a strongly deformed matrix of metasedimentary and mafic schists that encloses lesser-deformed blocks of metabasites,Carboniferous-Triassic metasedimentary rocks,and early Paleozoic *** the blocks and melange matrix exhibit greenschist,epidote-blueschist, and locally,epidote-amphibolite facies mineral *** reveals that the metamorphic belt experienced pressures of>10 *** equilibration temperatures for mafic schists in the melange matrix decrease from east to west,from～660℃near Shuang hu(33°N,89°E),～500℃near Rongma(33°N,87°E),to～425℃near Gangma Co(34°N,84°E).Equilibration at consistently high pressures over a large range of temperatures is compatible with metamorphism of Qiangtang melange within a low-angle subduction zone beneath a continental *** structural, thermobarometric,and Ar/39)Ar studies suggest that Qiangtang melange was exhumed in an intracontinental setting from depths of>35 km to upper crustal levels inhin the melange matrix yield U-Pb ion-microprobe ages that range from early Paleozoic to Early Archean,and could have been sourced from terranes to the north of the Jinsha *** results support a model in which Qiangtang melange was underthrust～200 km beneath the Qiangtang terrane during early Mesozoic flat-slab southward subduction of Paleo-Tethyan oceanic lithosphere along the Jinsha *** model predicts that significant portions of the central Tibetan continental mantle lithosphere were removed during early Mesozoic low-angle oceanic subduction and that the present-day central Tibetan deeper crust includes large volumes of underthrust early Mesozoic

关键词： Tibet blueschist melange exhumation subduction metamorphic core complex

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导弹与航天运载技术(中英文) 1987年第7期 13-26页

作者： Allan h.taylor 王亚文

可完全重复使用的运载火箭及在大气层中超高音速飞行的决定性技术是研制可重复使用的轻飞行重量的低温推进剂贮箱。本文介绍了对三种低温贮箱结构方案的研究分析结果(每种结构都悬挂在一个碳-碳航空壳结构中)。第一种贮箱方案是蜂窝夹... 详细信息

可完全重复使用的运载火箭及在大气层中超高音速飞行的决定性技术是研制可重复使用的轻飞行重量的低温推进剂贮箱。本文介绍了对三种低温贮箱结构方案的研究分析结果(每种结构都悬挂在一个碳-碳航空壳结构中)。第一种贮箱方案是蜂窝夹芯结构,夹芯中间保持真空进行绝热。第二种贮箱方案是整体加强蒙皮结构,采用低密度的、密封槽式低温泡沫进行绝热。第三种贮箱方案是非加强蒙皮结构,采用和第二种方案相同的泡沫绝热。评估了各种设计参数对贮箱重量的影响。贮箱结构主要根据气垫压力、液体静压力和空气惯性载荷的要求来确定。但也要考虑与推进剂的兼容性、断裂力学、热应力、最小蒙皮厚度约束条件及极限温度。本文还介绍了一些设计曲线,这些设计曲线反映了几种不同的设计参数对贮箱壁厚度的影响。利用这些设计曲线作为基本运载火箭可重复使用的轻飞行重量低温贮箱结构的分析工具。分析结果表明,压力稳定的、非加强蒙皮的、极限温度为400℉低温绝热铝贮箱,对于大多数的设计条件来说其重量是最小的。

关键词：大型火箭推进剂贮箱贮箱设计