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Tuning electronic structure of RuO_(2)by single atom Zn and oxygen vacancies to boost oxygen evolution reaction in acidic medium

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Journal of Energy Chemistry 2024年第1期88卷 94-102,I0003页

作者： Qing Qin Tiantian Wang Zijian Li Guolin Zhang Haeseong Jang Liqiang hou Yu Wang Min Gyu Kim shangguo Liu Xien Liu College of Chemical Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina Department of Chemistry City University of Hong KongHong Kong 999077China Department of Advanced Materials Engineering Chung-Ang UniversityAnseong-siGyeonggi-do 17546SeoulRepublic of Korea Beamline Research Division Pohang Accelerator Laboratory(PAL)Pohang 37673Gyeongsangbuk-doRepublic of Korea

The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers.To dramatically enhance the durability of RuO_(2)to construct activity-stability trade-off model is full of significance but challenging.Herein,a single atom Zn stabilized RuO_(2)with enriched oxygen vacancies(SA Zn-RuO_(2))is developed as a promising alternative to iridium oxide for acidic oxygen evolution reaction(OER).Compared with commercial RuO_(2),the enhanced Ru–O bond strength of SA Zn-RuO_(2)by forming Zn-O-Ru local structure motif is favorable to stabilize surface Ru,while the electrons transferred from Zn single atoms to adjacent Ru atoms protects the Ru active sites from overoxidation.Simultaneously,the optimized surrounding electronic structure of Ru sites in SA ZnRuO_(2)decreases the adsorption energies of OER intermediates to reduce the reaction barrier.As a result,the representative SA Zn-RuO_(2)exhibits a low overpotential of 210 mV to achieve 10 mA cm^(-2)and a greatly enhanced durability than commercial RuO_(2).This work provides a promising dual-engineering strategy by coupling single atom doping and vacancy for the tradeoff of high activity and catalytic stability toward acidic OER.

关键词： Electrocatalyst Acidic oxygen evolution reaction Electronic structure engineering Durability Reaction barrier

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Electron-deficient ZnO induced by heterointerface engineering as the dominant active component to boost CO_(2)-to-formate conversion

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Carbon Energy 2024年第5期6卷 127-136页

作者： Qing Qin Zijian Li Yingzheng Zhang Haeseong Jang Li Zhai Liqiang hou Xiaoqian Wei Zhe Wang Min Gyu Kim shangguo Liu Xien Liu College of Chemical Engineering Qingdao University of Science and TechnologyQingdaoChina Department of Chemistry City University of Hong KongHong Kong SARChina Department of Advanced Materials Engineering Chung-Ang UniversityAnseong-siGyeonggi-doRepublic of Korea Beamline Research Division Pohang Accelerator Laboratory(PAL)PohangRepublic of Korea

Electrocatalytic CO_(2)-to-formate conversion is considered an economically viable process.In general,Zn-based nanomaterials are well-known to be highly efficient electrocatalysts for the conversion of CO_(2) to CO,but seldom do they exhibit excellent selectivity toward formate.In this article,we demonstrate that a heterointerface catalyst ZnO/ZnSnO3 with nanosheet morphology shows enhanced selectivity with a maximum Faradaic efficiency(FE)of 86%at−0.9 V versus reversible hydrogen electrode and larger current density for the conversion of CO_(2) to formate than pristine ZnO and ZnSnO3.In particular,the FEs of the C1 products(CO+HCOO−)exceed 98%over the potential window.The experimental measurements combined with theoretical calculations revealed that the ZnO in ZnO/ZnSnO3 heterojunction delivers the valence electron depletion and accordingly optimizes Zn d-band center,which results in moderate Zn-O hybridization of HCOO*and weakened Zn-C hybridization of competing COOH*,thus greatly boosting the HCOOH generation.Our study highlights the importance of charge redistribution in catalysts on the selectivity of electrochemical CO_(2) reduction.

关键词： charge redistribution CO_(2)reduction reaction electrocatalyst heterointerfaces selectivity

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Structural and functional imaging of brains

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Science China Chemistry 2023年第2期66卷 324-366页

作者： Zhichao Liu Ying Zhu Liming Zhang Weiping Jiang Yawei Liu Qiaowei Tang Xiaoqing Cai Jiang Li Lihua Wang Changlu Tao Xianzhen Yin Xiaowei Li shangguo hou Dawei Jiang Kai Liu Xin Zhou Hongjie Zhang Maili Liu Chunhai Fan Yang Tian Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai200241China Interdisciplinary Research Center Shanghai Synchrotron Radiation FacilityZhangjiang LaboratoryShanghai Advanced Research InstituteChinese Academy of SciencesUniversity of Chinese Academy of SciencesShanghai201210China State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics Chinese Academy of SciencesWuhan National Laboratory for OptoelectronicsWuhan430071China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022China Department of Chemistry Tsinghua UniversityBeijing100084China School of Chemistry and Chemical Engineering Frontiers Science Center for Transformative MoleculesInstitute of Translational MedicineShanghai Jiao Tong UniversityShanghai200240China Interdisciplinary Center for Brain Information Brain Cognition and Brain Disease InstituteShenzhen-Hong Kong Institute of Brain Science-Shenzhen Fundamental Research InstitutionsFaculty of Life and Health SciencesShenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen518055China Lingang Laboratory Shanghai201602China School of Biomedical Engineering Shanghai Jiao Tong UniversityShanghai200240China Institute of Systems and Physical Biology Shenzhen Bay LaboratoryShenzhen518055China Department of Nuclear Medicine Union HospitalTongji Medical CollegeHuazhong University of Science and TechnologyWuhan430022China

Analyzing the complex structures and functions of brain is the key issue to understanding the physiological and pathological processes.Although neuronal morphology and local distribution of neurons/blood vessels in the brain have been known,the subcellular structures of cells remain challenging,especially in the live brain.In addition,the complicated brain functions involve numerous functional molecules,but the concentrations,distributions and interactions of these molecules in the brain are still poorly understood.In this review,frontier techniques available for multiscale structure imaging from organelles to the whole brain are first overviewed,including magnetic resonance imaging(MRI),computed tomography(CT),positron emission tomography(PET),serial-section electron microscopy(ss EM),light microscopy(LM)and synchrotron-based X-ray microscopy(XRM).Specially,XRM for three-dimensional(3D)imaging of large-scale brain tissue with high resolution and fast imaging speed is highlighted.Additionally,the development of elegant methods for acquisition of brain functions from electrical/chemical signals in the brain is outlined.In particular,the new electrophysiology technologies for neural recordings at the single-neuron level and in the brain are also summarized.We also focus on the construction of electrochemical probes based on dual-recognition strategy and surface/interface chemistry for determination of chemical species in the brain with high selectivity and long-term stability,as well as electrochemophysiological microarray for simultaneously recording of electrochemical and electrophysiological signals in the brain.Moreover,the recent development of brain MRI probes with high contrast-to-noise ratio(CNR)and sensitivity based on hyperpolarized techniques and multi-nuclear chemistry is introduced.Furthermore,multiple optical probes and instruments,especially the optophysiological Raman probes and fiber Raman photometry,for imaging and biosensing in live brain are emphasized.Finally,a brief perspective on existing cha

关键词： brain structure brain function brain chemistry chemical signal biosensing and bioimaging

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Superresolution imaging of telomeres with continuous wave stimulated emission depletion (STED) microscope

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Science China Chemistry 2016年第11期59卷 1519-1524页

作者： Shaopeng Wang Suhui Deng Xiaoqing Cai shangguo hou Jiajun Li Zhaoshuai Gao Jiang Li Lihua Wang Chunhai Fan Division of Physical Biology&Bioimaging Center Shanghai Synchrotron Radiation FacilityCAS Key Laboratory of Interfacial Physics and TechnologyShanghai Institute of Applied PhysicsChinese Academy of SciencesShanghai 201800China University of Chinese Academy of Sciences Beijing 100049China School of Information Engineering Nanchang UniversityNanchang 330031China

The significant role of telomeres in cells has attracted much attention since they were discovered.Fluorescence imaging is an effective method to study subcellular structures like telomeres.However,the diffraction limit of traditional optical microscope hampers further investigation on them.Recent progress on superresolution fluorescence microscopy has broken this limit.In this work,we used stimulated emission depletion(STED) microscope to observe fluorescence-labeled telomeres in interphase cell nuclei.The results showed that the size of fluorescent puncta representing telomeres under the STED microscope was much smaller than that under the confocal microscope.Two adjacent telomeres were clearly separated via STED imaging,which could hardly be discriminated by confocal microscopy due to the diffraction limit.We conclude that STED microscope is a more powerful tool that enable us to obtain detailed information about telomeres.

关键词： telomere superresolution 成像刺激排放弄空(STED ) 显微镜学在 situ 杂交(鱼) 的荧光

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磷掺杂碳负载Zn_(x)P_(y)O_(z)常温常压下高效电催化合成氨

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物理化学学报 2024年第3期40卷 29-30页

作者：王佳秦清王哲赵旭浩陈云菲候利强刘尚果刘希恩青岛科技大学化工学院山东青岛266042

合成氨(NH_(3))的发展是现代工业进程和人类生存的基石。受氮气(N_(2))化学惰性的限制,当前的合成氨工业能源消耗高并且排放大量的二氧化碳。电化学氮气还原反应(NRR),是有望取代高能耗的Haber-Bosch(HB)合成法的一种绿色可持续的合成... 详细信息

合成氨(NH_(3))的发展是现代工业进程和人类生存的基石。受氮气(N_(2))化学惰性的限制,当前的合成氨工业能源消耗高并且排放大量的二氧化碳。电化学氮气还原反应(NRR),是有望取代高能耗的Haber-Bosch(HB)合成法的一种绿色可持续的合成氨工艺。然而,因氮气以及析氢竞争富反应(HER)导致电催化氮气还原极低的NH_(3)产率和能量转换效率一直是目前人工固氮领域面临的挑战。在本文中,我们报道了一种具有丰富孔结构的磷掺杂碳(PC)负载Zn_(3)(PO_(4))_(2)/Zn_(2)P_(2)O_(7)纳米复合材料(h-PC/Zn_(3)(PO_(4))_(2)/Zn_(2)P_(2)O_(7)),在酸性和中性介质中将N_(2)高效催化转化为NH_(3)。其独特的分级多孔结构提高了表面粗糙度并加快了氮气在催化剂体相中的扩散,这有利于延长氮气在催化剂表面的停留时间以及提高活性位点的利用效率。而多组分的均匀分布可以调节电子结构并优化反应中间体的吸附行为,进而提高活性位点的本征活性。在0.1mol·L^(-1)HCI电解液中,h-PC/Zn_(3)(PO_(4))_(2)/Zn_(2)P_(2)O_(7)在-0.2 V vs.可逆氢电极(RHE)电位下NH_(3)的产率可以达到38.7±1.2μg·h^(-1)·mgcat^(-1),法拉第效率为19.8%±0.9%。此外;h-PC/Zn_(3)(PO_(4))_(2)/Zn_(2)P_(2)O_(7)在0.1 mol·L^(-1)Na_(2)SO_(4)溶液中同样展现出优异的电催化氮气还原合成氨性能,NH_(3)产率及法拉第效率分别为17.1±0.8μg·h^(-1)·mgcat^(-1)和15.g%±0.6%,明显优于PC/Zn_(3)P_(2)、C/ZnO和大多数报道的非贵金属电催化剂。这种优异的性能主要归因于多孔结构有利于传质及多组分活性位点协同效应。此外,我们采用非原位X射线光电子能谱(XPS)、透射电子显微镜(TEM)和X射线衍射(XRD)等表征手段对NRR测试前后h-PC/Zn_(3)(PO_(4))_(2)/Zn_(2)P_(2)O_(7)的组成和结构变化进行了剖析。在反应后检测到了新增的N物种信号,证明催化剂确实发生了氮气还原反应。本研究提供了一种通过同步构建传质通道并耦合不同的活性位点以协同增强NRR活性和选择性的新思路,这对加快绿色制氨工业化具有重大意义。

关键词：氮气还原反应电催化剂孔结构多活性中心协同效应

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Nanoprobes for super-resolution fluorescence imaging at the nanoscale

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Science China Chemistry 2014年第1期57卷 100-106页

作者： hou shangguo LIANG Le DENG SuHui CHEN JianFang HUANG Qing CHENG Ya FAN ChunHai Division of Physical Biology and Bioimaging Center Shanghai Synchrotron Radiation Facility Shanghai Institute of Applied Physics Chinese Academy of Sciences Shanghai Institute of Optics and Fine Mechanics Chinese Academy of Sciences

Compared with other imaging techniques,fluorescence microscopy has become an essential tool to study cell biology due to its high compatibility with living cells.Owing to the resolution limit set by the diffraction of light,fluorescence microscopy could not resolve the nanostructures in the range of<200 nm.Recently,many techniques have been emerged to overcome the diffraction barrier,providing nanometer spatial resolution.In the course of development,the progress in fluorescent probes has helped to promote the development of the high-resolution fluorescence nanoscopy.Here,we describe the contributions of the fluorescent probes to far-field super resolution imaging,focusing on concepts of the existing super-resolution nanoscopy based on the photophysics of fluorescent nanoprobes,like photoswitching,bleaching and blinking.Fluorescent probe technology is crucial in the design and implementation of super-resolution imaging methods.

关键词： super-resolution microscopy,diffraction barrier,switching characteristic

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Mass spectrometry imaging and single-cell transcriptional profiling reveal the tissue-specific regulation of bioactive ingredient biosynthesis in Taxus leaves

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Plant Communications 2023年第5期4卷 29-45页

作者： Xiaori Zhan Tian Qiu Hongshan Zhang Kailin hou Xueshuang Liang Cheng Chen Zhijing Wang Qicong Wu Xiaojia Wang Xiao-lin Li Mingshuang Wang shangguo Feng houqing Zeng Chunna Yu Huizhong Wang Chenjia Shen College of Life and Environmental Sciences Hangzhou Normal UniversityHangzhou 311121China Zhejiang Provincial Key Laboratory for Genetic Improvement and Quality Control of Medicinal Plants Hangzhou Normal UniversityHangzhou 311121China Kharkiv Institute Hangzhou Normal UniversityHangzhou 311121China College of Pharmacy Hangzhou Normal UniversityHangzhou 311121China State Key Laboratory Breeding Base of Dao-di Herbs National Resource Center for Chinese Materia MedicaChina Academy of Chinese Medical SciencesBeijing 100700China

Taxus leaves provide the raw industrial materials for taxol,a natural antineoplastic drug widely used in the treatment of various cancers.However,the precise distribution,biosynthesis,and transcriptional regulation of taxoids and other active components in Taxus leaves remain unknown.Matrix-assisted laser desorption/ionization–mass spectrometry imaging analysis was used to visualize various secondary metabolites in leaf sections of Taxus mairei,confirming the tissue-specific accumulation of different active metabolites.Single-cell sequencing was used to produce expression profiles of 8846 cells,with a median of 2352 genes per cell.Based on a series of cluster-specific markers,cells were grouped into 15 clusters,suggesting a high degree of cell heterogeneity in T.mairei leaves.Our data were used to create the first Taxus leaf metabolic single-cell atlas and to reveal spatial and temporal expression patterns of several secondary metabolic pathways.According to the cell-type annotation,most taxol biosynthesis genes are expressed mainly in leaf mesophyll cells;phenolic acid and flavonoid biosynthesis genes are highly expressed in leaf epidermal cells(including the stomatal complex and guard cells);and terpenoid and steroid biosynthesis genes are expressed specifically in leaf mesophyll cells.A number of novel and cell-specific transcription factors involved in secondary metabolite biosynthesis were identified,including MYB17,WRKY12,WRKY31,ERF13,GT_2,and bHLH46.Our research establishes the transcriptional landscape of major cell types in T.mairei leaves at a single-cell resolution and provides valuable resources for studying the basic principles of cell-type-specific regulation of secondary metabolism.

关键词： scRNA-seq taxol biosynthesis Taxus mairei secondary metabolism transcription regulation

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河北武安玉石洼铁矿中磁铁矿特征及其对铁矿床成因指示意义

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地学前缘 2019年第6期26卷 244-256页

作者：侯晓阳苏尚国杨跃跃中国地质大学(北京)地球科学与资源学院

夕卡岩铁矿床的成因一直以来备受争议,主要有接触交代和矿浆成因等模型。河北武安玉石洼铁矿是邯邢地区主要的夕卡岩铁矿之一,对矿区尖山剖面中的三类磁铁矿成分进行详细研究有助于解决此问题。产于剖面下部玉石洼铁矿主矿体中的磁铁矿... 详细信息

夕卡岩铁矿床的成因一直以来备受争议,主要有接触交代和矿浆成因等模型。河北武安玉石洼铁矿是邯邢地区主要的夕卡岩铁矿之一,对矿区尖山剖面中的三类磁铁矿成分进行详细研究有助于解决此问题。产于剖面下部玉石洼铁矿主矿体中的磁铁矿以高Ti为特征,而在上部结晶灰岩中矿脉状中磁铁矿以高Si(w(SiO2)>1%)为特点,赋存于中部二长岩矿脉中的磁铁矿具有过渡的成分特征。通过对此三类磁铁矿中主量元素、微量元素研究发现,从下部玉石洼主矿体向上部结晶灰岩中的磁铁矿脉,磁铁矿具有Ti含量逐渐减少而Si、Mg含量逐渐增加的特征。高硅磁铁矿呈自形晶,与方解石平衡共生,其形成与流体有关,很可能是流体晶矿物。磁铁矿Fe-V/Ti判别图解显示下部玉石洼主矿体中部分磁铁矿具有岩浆成因,二长岩和结晶灰岩中的脉状矿石中磁铁矿具有热液成因,磁铁矿由下部到上部具有岩浆成因过渡为热液成因的连续过程。根据玉石洼矿区磁铁矿的这些特征,我们认为铁矿浆中含有大量流体,应该为"含铁熔体-流体",由于流体超压使"含铁熔体-流体流"在岩浆通道中快速上升,至地壳浅部空间就位,在空间上由下部形成高温高Ti磁铁矿过渡为上部形成具有流体晶特征的高Si磁铁矿的岩浆通道成矿系统模型。

关键词：邯邢铁矿高钛磁铁矿高硅磁铁矿含矿熔体-流体流岩浆通道成矿系统

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内蒙温根南基性-超基性岩体岩石学、地球化学特征及其形成构造背景

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岩石学报 2014年第12期30卷 3729-3740页

作者：侯建光苏尚国周岱王倩中国地质大学地球科学与资源学院北京100083 中国地质调查局武汉地质调查中心武汉541000

内蒙古温根南岩体位于内蒙古中部,属于华北克拉通北缘中段,主要火成岩组合为纯橄岩-橄长岩-辉长岩,平面上呈NNE向延伸。元素地球化学分析结果显示,岩体富Mg、低碱和Ti O2,全岩氧化物含量主要受控于橄榄石、单斜辉石和斜长石的相对分配比... 详细信息

内蒙古温根南岩体位于内蒙古中部,属于华北克拉通北缘中段,主要火成岩组合为纯橄岩-橄长岩-辉长岩,平面上呈NNE向延伸。元素地球化学分析结果显示,岩体富Mg、低碱和Ti O2,全岩氧化物含量主要受控于橄榄石、单斜辉石和斜长石的相对分配比例,微量元素含量总体较低,具Nb、Ta和Hf轻微亏损,Pb、Sr显著富集的特征。其中辉长岩表现出显著的Nb、Ta负异常和Pb、Sr正异常。辉长岩微量元素相对纯橄岩和橄长岩明显富集。辉长岩相-纯橄岩相中总稀土含量变化较大（1.41×10-6~111.6×10-6）,稀土元素配分曲线表现为轻微右倾型与平坦型,岩体深部超基性岩类总稀土含量极低,随着其结晶分异程度的增大和堆晶作用的加强,岩石中稀土元素含量迅速升高,反映晶间残余熔体的比重不断升高。运用橄榄石与残余熔浆平衡方法制约母岩浆性质,结果表明温根南岩体初始岩浆MgO=11.73%,FeO=11.38%,属于高镁玄武质岩浆。温根南岩体基性-超基性岩中Sr-Nd同位素投点主要靠近EM I型富集地幔端元,推测幔源岩浆在源区或上升过程中受到了地壳物质的混染。运用Zr、Y、Th、Ta等不相容元素的比值（判别岩浆演化过程,基于Th/Nb比值（〉1）和低Nb/La比值（〈1）表明温根南岩体初始岩浆侵位过程中遭受到了地壳物质的混染。温根南岩体Ta/Th-Zr/Nb、Th/Yb-Th/Nb、Ta/Th-Th/Yb、Nb/Th-Nb构造环境判别图中主要落入板内玄武岩（WPB）范围,推测温根南基性-超基性岩体在早石炭纪形成于板内伸展构造环境。

关键词：温根南基性-超基性岩地球化学特征岩浆源区母岩浆性质内蒙

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基于时间门技术的纳米显微镜原理及应用

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中国科学：化学 2015年第11期45卷 1206-1213页

作者：侯尚国王坤王丽华黄庆邓素辉中国科学院上海应用物理研究所物理生物学研究室上海201800

很久以来,光学显微镜的分辨率受限于光学衍射极限.最近几年,发展了很多突破光学衍射极限的技术方法.其中,受激发射损耗(stimulated emission depletion,STED)显微镜因能够提供超快超高的分辨率而备受关注.在这类方法中,脉冲式STED分辨... 详细信息

很久以来,光学显微镜的分辨率受限于光学衍射极限.最近几年,发展了很多突破光学衍射极限的技术方法.其中,受激发射损耗(stimulated emission depletion,STED)显微镜因能够提供超快超高的分辨率而备受关注.在这类方法中,脉冲式STED分辨率较高但搭建复杂;连续光STED虽然搭建简单,但分辨率有所下降;时间门调制STED(gated-STED,g STED)在简化STED搭建的同时,又可以实现与脉冲式STED相比拟的分辨率.本文详细介绍了时间门在STED纳米显微镜中的应用.

关键词：超分辨成像时间门纳米显微镜受激发射损耗显微镜

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