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cryo-electron microscopy structure of the intact photosynthetic light-harvesting antenna-reaction center complex from a green sulfur bacterium

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Journal of Integrative Plant Biology 2023年第1期65卷 223-234页

作者： Jing-Hua Chen Weiwei Wang Chen Wang Tingyun Kuang Jian-Ren Shen Xing Zhang College of Life Science Zhejiang University Hangzhou 310058 China Department of Pathology of Sir Run Run Shaw Hospital and Department of Biophysics Zhejiang University School of MedicineHangzhou 310058 China Key Laboratory of Photobiology Institute of BotanyPhotosynthesis Research Center the Chinese Academy of SciencesBeijing 100093 China Research Institute for Interdisciplinary Science and Graduate School of Natural Science and Technology Okayama UniversityOkayama 700-8530 Japan center of cryo electron microscopy Zhejiang University School of Medicine Hangzhou 310058 China

The photosynthetic reaction center complex(RCC)of green sulfur bacteria(GSB)consists of the membrane-imbedded RC core and the peripheric energy transmitting proteins called Fenna–Matthews–Olson(FMO).Functionally,FMO transfers the absorbed energy from a huge peripheral light-harvesting antenna named chlorosome to the RC core where charge separation occurs.In vivo,one RC was found to bind two FMOs,however,the intact structure of RCC as well as the energy transfer mechanism within RCC remain to be clarified.Here we report a structure of intact RCC which contains a RC core and two FMO trimers from a thermophilic green sulfur bacterium Chlorobaculum tepidum at 2.9A resolution by cryo-electron microscopy.The second FMO trimer is attached at the cytoplasmic side asymmetrically relative to the first FMO trimer reported previously.We also observed two new subunits(PscE and PscF)and the N-terminal transmembrane domain of a cytochrome-containing subunit(PscC)in the structure.These two novel subunits possibly function to facilitate the binding of FMOs to RC core and to stabilize the whole complex.A new bacteriochlorophyll(numbered as 816)was identified at the interspace between PscF and PscA-1,causing an asymmetrical energy transfer from the two FMO trimers to RC core.Based on the structure,we propose an energy transfer network within this photosynthetic apparatus.

关键词： cryo-electron microscopy energy transfer FMO protein green sulfur bacterium photosynthesis reaction center

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Efficient optimization of electron transfer pathway by constructing phosphide/ceria interface boosts seawater hydrogen production

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Journal of Energy Chemistry 2024年第8期95卷 490-498页

作者： Yifan Zhao Lingfeng Yang Youyu Long Min Xi Anran Chen Hua Zhang School of Materials and Energy Yunnan University electron microscopy Centre of Yunnan University Yunnan University

Developing efficient and durable hydrogen evolution reaction（HER） electrocatalysts is one of the most important issues for the commercialization of seawater electrolysis,but it remains challenging.Here,we report a CeO2-CoP nanoneedle array catalyst loaded on Ti mesh（CeO2-CoP/TM） with workfunction-induced directional charge transport properties.The CeO2-CoP/TM catalyst showed superior HER catalytic activity and stability,with over potentials of 41 and 60 mV to attain 10 mA cm-2,in 1 M KOH and 1 M KOH+seawater electrolyte,respectively.Experimental results and theoretical calculations reveal that the work function drives the charge transfer from CeO2to CoP,which effectively balances the electronic density of CoP and CeO2,optimizes the d-band center,and accelerates the water activation kinetics,thus enhancing the HER activity.The solar-driven water electrolysis device displays a high and stable solar-to-hydrogen conversion efficiency of 19.6%.This study offers a work function-induced directional charge transport strategy to design efficient and durable catalysts for hydrogen production.

关键词： Charge transport Heterostructure Seawater splitting Solar-to-hydrogen Work function

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Optimizing high-coordination shell of Co-based single-atom catalysts for efficient ORR and zinc-air batteries

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Journal of Energy Chemistry 2024年第8期95卷 306-314页

作者： Yugang Qi Qing Liang Kexin Song Xinyan Zhou Meiqi Liu Wenwen Li Fuxi Liu Zhou Jiang Xu Zou Zhongjun Chen Wei Zhang Weitao Zheng Key Laboratory of Automobile Materials MOE School of Materials Science & Engineering Electron Microscopy Center and International Center of Future Science Jilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy Materials Jilin University Institute of High Energy Physics Chinese Academy of Sciences

Atom-level modulation of the coordination environment for single-atom catalysts(SACs) is considered as an effective strategy for elevating the catalytic performance. For the MNxsite, breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way, but it remains challenging for elucidating the underlying mechanism of interaction. Herein, a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks. X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell(denoted as Co-N/P-C).The prepared catalyst exhibits excellent oxygen reduction reaction(ORR) activity as well as zinc-air battery performance. The introduction of P atoms in the Co-SACs weakens the interaction between Co and N,significantly promoting the adsorption process of *OOH, resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier, responsible for the increased intrinsic activity. Our discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion.

关键词： Electrocatalytic Oxygen reduction reaction Shell coordination optimization Single atom catalyst

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Hierarchical FeO_(χ)H_(y)@Ni_(3)B hybrid for efficient alkaline oxygen evolution at high current density

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Journal of Energy Chemistry 2024年第7期94卷 599-607页

作者： Fuxi Liu Qing Liang Zhenyu Li Meiqi Liu Naiin Yue Zizhun Wang Xu Zou Wei Zhang Key Laboratory of Automobile Materials Ministry of Education School of Materials Science&EngineeringElectron Microscopy CenterInternational Center of Future ScienceJilin Provincial International Cooperation Key Laboratory of High-Eficiency Clean Energy MaterialsJilin UniversityChangchun 130012JilinChina

Electrocatalysts with high activity and long-term durability are vital toward large-scale hydrogen pro-duction from electrocatalytic water splitting.Here,the self-supported electrode(FeO_(χ)H_(y)@Ni_(3)B/NF)with hierarchical heterostructure was simply prepared by using NigB chunks grown on nickel foam as sub-strate to in situ form vertical FeO_(χ)H_(y)nanosheets.Such hybrid shows efficient oxygen evolution reaction activity with overpotentials as low as 267 and 249 mV at 100 mA cm^(-2)in 1 M K0H solution and 30 wt%KOH solution,respectively.Meanwhile,it also exhibits excellent catalytic stability,sustaining catalysis at 500 mA cm^(-2)in 1 M K0H solution for 200 h,and even for 200 h at 1000 mA cm^(-2)in 30 wt%K0H solution.Further experimental results reveal that the FeO_(χ)H_(y)@Ni_(3)B/NF is endowed with superhydrophilic and superaerophobic surface properties,which not only provide more mass transport channels,as well as facilitated the diffusion of reaction intermediates and gas bubbles.Also,it holds faster reaction kinetics,more accessible active sites and accelerated electron transfer rates due to strong synergistic interactions attheheterogeneous interface.

关键词： FeO_(χ)H_(y)@Ni_(3)B/NF hybrid Heterostructure Oxygen evolution reaction Electrocatalytic

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High-efficiency sodium storage of Co_(0.85)Se/WSe_(2) encapsulated in N-doped carbon polyhedron via vacancy and heterojunction engineering

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Carbon Energy 2024年第1期6卷 94-107页

作者： Ya Ru Pei Hong Yu Zhou Ming Zhao Jian Chen Li Xin Ge Wei Zhang Chun Cheng Yang Qing Jiang Key Laboratory of Automobile Materials(Jilin University) Ministry of EducationSchool of Materials Science and EngineeringJilin UniversityChangchunChina Jilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy Materials Electron Microscopy CenterJilin UniversityChangchunChina

With the advantage of fast charge transfer,heterojunction engineering is identified as a viable method to reinforce the anodes'sodium storage performance.Also,vacancies can effectively strengthen the Na+adsorption ability and provide extra active sites for Na+adsorption.However,their synchronous engineering is rarely reported.Herein,a hybrid of Co_(0.85)Se/WSe_(2) heterostructure with Se vacancies and N-doped carbon polyhedron(CoWSe/NCP)has been fabricated for the first time via a hydrothermal and subsequent selenization strategy.Spherical aberration-corrected transmission electron microscopy confirms the phase interface of the Co_(0.85)Se/WSe_(2) heterostructure and the existence of Se vacancies.Density functional theory simulations reveal the accelerated charge transfer and enhanced Na+adsorption ability,which are contributed by the Co_(0.85)Se/WSe_(2) heterostructure and Se vacancies,respectively.As expected,the CoWSe/NCP anode in sodium-ion battery achieves outstanding rate capability(339.6 mAh g^(−1) at 20 A g^(−1)),outperforming almost all Co/W-based selenides.

关键词： Co_(0.85)Se/WSe_(2)heterostructure density functional theory simulations N-doped carbon polyhedron Se vacancies sodium-ion batteries

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Ultra-thin robust CNT@GC film integrating effective electromagnetic shielding and flexible Joule heating

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Nano Research 2024年第5期17卷 3462-3471页

作者： Ding Zhang Chunhui Wang Meng Li Weixue Meng Shipeng Zhang Mengdan Yang Xinguang Huang Yingjiu Zhang Yuanyuan Shang Anyuan Cao Key Laboratory of Materials Physics(Ministry of Education) School of Physics and MicroelectronicsZhengzhou UniversityZhengzhou450052China electron microscopy center Yunnan UniversityKunming650091China School of Materials Science and Engineering Peking UniversityBeijing100871China

The demand for lightweight,thin electromagnetic interference(EMI)shielding film materials with high shielding effectiveness(SE),excellent mechanical properties,and stability in complex environments is particularly pronounced in the realm of flexible and portable electronic products.Here,we developed an ultra-thin film(CNT@GC)in which the glassy carbon(GC)layer wrapped around and welded carbon nanotubes(CNTs)to form a core-shell network structure,leading to exceptional tensile strength(327.2 MPa)and electrical conductivity(2.87×10^(5) S·m^(−1)).The CNT@GC film achieved EMI SE of 60 dB at a thickness of 2µm after post-acid treatment and high specific SE of 3.49×10^(5) dB·cm^(2)·g^(−1),with comprehensive properties surpassing those of the majority of previous shielding materials.Additionally,the CNT@GC film exhibited Joule heating capability,reaching a surface temperature of 135℃at 3 V with a fast thermal response of about 0.5 s,enabling anti-icing/de-icing functionality.This work presented a methodology for constructing a robust CNT@GC film with high EMI shielding performance and exceptional Joule heating capability,demonstrating immense potential in wearable devices,defense,and aerospace applications.

关键词： core-shell structure ultra-thin lightweight film robust film electromagnetic shielding Joule heating

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High-performance terahertz modulators induced by substrate field in Te-based all-2D heterojunctions

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Light(Science & Applications) 2024年第3期13卷 577-586页

作者： Pujing Zhang Qihang Liang Qingli Zhou Jinyu Chen Menglei Li Yuwang Deng Wanlin Liang Liangliang Zhang Qinghua Zhang Lin Gu Chen Ge Kui-juan Jin Cunlin Zhang Guozhen Yang Department of Physics Key Laboratory of Terahertz OptoelectronicsMinistry of Educationand Beijing Advanced Innovation Center for Imaging Theory and TechnologyCapital Normal UniversityBeijing 100048China Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China Department of Materials Science and Engineering Beijing National Center for Electron Microscopy and Laboratory of Advanced MaterialsTsinghua UniversityBeijing 100084China

High-performance active terahertz modulators as the indispensable core components are of great importance for the next generation communication technology.However,they currently suffer from the tradeoff between modulation depth and speed.Here,we introduce two-dimensional(2D)tellurium(Te)nanofilms with the unique structure as a new class of optically controlled terahertz modulators and demonstrate their integrated heterojunctions can successfully improve the device performances to the optimal and applicable levels among the existing all-2D broadband modulators.Further photoresponse measurements confirm the significant impact of the stacking order.We first clarify the direction of the substrate-induced electric field through first-principles calculations and uncover the unusual interaction mechanism in the photoexcited carrier dynamics associated with the charge transfer and interlayer exciton recombination.This advances the fundamental and applicative research of Te nanomaterials in high-performance terahertz optoelectronics.

关键词： performance field terahertz

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Kinetically and thermodynamically expediting elementary steps via high-valence Cr-incorporated of nickel selenide for water electrolysis

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Nano Research 2024年第3期17卷 1199-1208页

作者： Huafeng Fan Dongxu Jiao Jinchang Fan Dewen Wang Bilal Zaman Wei Zhang Lei Zhang Weitao Zheng Xiaoqiang Cui State Key Laboratory of Automotive Simulation and Control School of Materials Science and EngineeringKey Laboratory of Automobile Materials of MOEJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsElectron Microscopy CenterJilin UniversityChangchun 130012China College of Chemistry Jilin UniversityChangchun 130012China

Designing high-performance electrocatalysts toward hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is essential to reduce the activation barrier and optimize free adsorption energy of reactive intermediates.Herein,we report that incorporating high-valence Cr into NiSe_(2)(Cr_(x)Ni_(1-x)Se_(2))kinetically and thermodynamically expedites elementary steps of both HER and OER.The as-prepared Cr_(0.05)Ni_(0.95)Se_(2) catalyst displays excellent HER and OER activities,with low overpotentials of 89 and 272 mV at the current density of 10 mA·cm^(-2)(j10),respectively,and remains stable during operation for 30 h.A low cell voltage of only 1.59 V is required to drive j10 in alkaline media.In situ Raman spectroscopy reveals that Cr incorporation facilitates the formation of NiOOH active species during the OER process.Meanwhile,theoretical explorations demonstrate that high-valence Cr incorporation efficiently accelerates water dissociation kinetics and improves H*adsorption during HER process,lowering the activation barrier of OER and optimizing the adsorption energy of oxygen-based intermediate,thus kinetically and thermodynamically enhancing the intrinsic performance of NiSe_(2) for over water splitting.This strategy provides a new horizon to design transition metal based electrocatalysts in the clean energy field.

关键词： nickel selenide electrocatalytic water splitting high-valence Cr density functional theory(DFT)calculation

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Cu/Mo2C synthesized through Anderson-type polyoxometalates modulate interfacial water structure to achieve hydrogen evolution at high current density

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Nano Research 2024年第4期17卷 2546-2554页

作者： Dunyuan Jin Fen Qiao Yan Zhou Junfeng Wang Kecheng Cao Jing Yang Jikang Zhao Lei Zhou Haitao Li School of Energy and Power Engineering Jiangsu UniversityZhenjiang 212013China School of Physical Science and Technology and Shanghai Key Laboratory of High-resolution electron microscopy ShanghaiTech UniversityShanghai 201210China Institute for Energy Research Jiangsu UniversityZhenjiang 212013China

The development of efficient non-precious metal catalysts is important for the large-scale application of alkaline hydrogen evolution reaction(HER).Here,we synthesized a composite catalyst of Cu and Mo_(2)C(Cu/Mo_(2)C)using Anderson-type polyoxometalates(POMs)synthesized by the facile soaking method as precursors.The electronic interaction between Cu and Mo_(2)C drives the positive charge of Cu,alleviating the strong adsorption of hydrogen at the Mo site by modulating the d-band center of Mo_(2)C.By studying the interfacial water structure using in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS),we determined that the positively charged Cu crystals have the function of activating water molecules and optimizing the interfacial water structure.The interfacial water of Cu/Mo_(2)C contains a large amount of free water,which could facilitate the transport of reaction intermediates.Due to activated water molecules and optimized interfacial water structure and hydrogen adsorption energy,the overpotential of Cu/Mo_(2)C is 24 mV at a current density of 10 mA·cm^(-2) and 178 mV at a current density of 1000 mA·cm^(-2).This work improves catalyst performance in terms of interfacial water structure optimization and deepens the understanding of water-mediated catalysis.

关键词： electrocatalytic hydrogen production interfacial water charge transport d band center in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)

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The structure of HSV-1 gB bound to a potent neutralizing antibody reveals a conservative antigenic domain across herpesviruses

hLife

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hLife 2024年第3期2卷 141-146页

作者： Cong Sun Jia-Wen Yang Chu Xie Xin-Yan Fang Guo-Long Bu Ge-Xin Zhao Dan-Ling Dai Zheng Liu Mu-Sheng Zeng State Key Laboratory of Oncology in South China Guangdong Key Laboratory of Nasopharyngeal Carcinoma Diagnosis and TherapyGuangdong Provincial Clinical Research Center for CancerSun Yat-sen University Cancer CenterGuangdongChina cryo-electron microscopy center Southern University of Science and TechnologyGuangdongChina Department of Biology Southern University of Science and TechnologyGuangdongChina

Human herpesviruses(HHV),including the alpha,beta,andgamma subfamilies,are enveloped viruses with broad prevalence,establishing life-time latent infections and inducing a variety of diseases[1].Among them,herpes simplex virus(HSV),consists of two HSV-1 and HSV-2 variants,ubiquitouslyaffecting global populations[2].As an enveloped virus,HSV features a repertoire of glycoproteins such as glycoproteins D(gD),glycoproteins H(gH),glycoproteins L(gL),and glycoproteins B(gB),to orchestrate host cell recognition and infection[3,4].

关键词： diseases neutral envelope

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