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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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Heterostructure Cu_(3)P-Ni_(2)P/CP catalyst assembled membrane electrode for high-efficiency electrocatalytic nitrate to ammonia

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Nano Research 2024年第6期17卷 4872-4881页

作者： Meng Jin Jiafang Liu Xian Zhang Shengbo Zhang Wenyi Li Dianding Sun Yunxia Zhang guozhong wang 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 PhysicsHefei Institutes of Physical ScienceChinese Academy of SciencesHefei 230031China University of Science and Technology of China Hefei 230026China Anhui Contango New Energy Technology Co. Ltd.Hefei 230031China

Electrochemical nitrate reduction reaction(NO_(3)RR)is a promising means for generating the energy carrier ammonia.Herein,we report the synthesis of heterostructure copper-nickel phosphide electrocatalysts via a simple vapor-phase hydrothermal method.The resultant catalysts were evaluated for electrocatalytic nitrate reduction to ammonia(NH_(3))in three-type electrochemical reactors.In detail,the regulation mechanism of the heterogeneous Cu_(3)P-Ni_(2)P/CP-x for NO_(3)RR performance was systematically studied through the H-type cell,rotating disk electrode setup,and membrane-electrode-assemblies(MEA)electrolyzer.As a result,the Cu_(3)P-Ni_(2)P/CP-0.5 displays the practicability in an MEA system with an anion exchange membrane,affording the largest ammonia yield rate(RNH_(3))of 1.9 mmol·h^(−1)·cm^(−2),exceeding most of the electrocatalytic nitrate reduction electrocatalysts reported to date.The theoretical calculations and in-situ spectroscopy characterizations uncover that the formed heterointerface in Cu_(3)P-Ni_(2)P/CP is beneficial for promoting nitrate adsorption,activation,and conversion to ammonia through the successive hydrodeoxygenation pathway.

关键词： electrocatalytic nitrate reduction to ammonia three-type reactors membrane-electrode-assemblies system operando ATR-IRRAS successive hydrodeoxygenation pathway

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Weakly Polarized Organic Cation-Modified Hydrated Vanadium Oxides for High-Energy Efficiency Aqueous Zinc-Ion Batteries

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Nano-Micro Letters 2024年第7期16卷 169-186页

作者： Xiaoxiao Jia Chaofeng Liu Zhi wang Di Huang guozhong Cao Department of Materials Science and Engineering University of WashingtonSeattleWA 98195USA School of Materials Science and Engineering Tongji UniversityShanghai 201804People’s Republic of China

Vanadium oxides,par-ticularly hydrated forms like V_(2)O_(5)·nH_(2)O(VOH),stand out as promising cathode candidates for aqueous zinc ion batteries due to their adjustable layered structure,unique electronic characteristics,and high theoretical capacities.However,challenges such as vanadium dissolution,sluggish Zn^(2+)diffusion kinetics,and low operating voltage still hinder their direct application.In this study,we present a novel vanadium oxide([C_(6)H_(6)N(CH_(3))_(3)]_(1.08)V_(8)O_(20)·0.06H_(2)O,TMPA-VOH),developed by pre-inserting trimethylphenylammonium(TMPA+)cations into VOH.The incorporation of weakly polarized organic cations capitalizes on both ionic pre-intercalation and molecular pre-intercalation effects,resulting in a phase and morphology transition,an expansion of the interlayer distance,extrusion of weakly bonded interlayer water,and a substantial increase in V^(4+)content.These modifications synergistically reduce the electrostatic interactions between Zn^(2+)and the V-O lattice,enhancing structural stability and reaction kinetics during cycling.As a result,TMPA-VOH achieves an elevated open circuit voltage and operation voltage,exhibits a large specific capacity(451 mAh g^(-1)at 0.1 A g^(-1))coupled with high energy efficiency(89%),the significantly-reduced battery polarization,and outstanding rate capability and cycling stability.The concept introduced in this study holds great promise for the development of high-performance oxide-based energy storage materials.

关键词： Zinc-ion battery Vanadium oxide V_(2)O_(5)·nH_(2)O Pre-intercalation Interlayer engineering

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Efficient single‑pixel imaging based on a compact fiber laser array and untrained neural network

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Frontiers of Optoelectronics 2024年第1期17卷 85-93页

作者： Wenchang Lai guozhong Lei Qi Meng Yan wang Yanxing Ma Hao Liu Wenda Cui Kai Han College of Advanced Interdisciplinary Studies National University of Defense TechnologyChangsha 410073China Nanhu Laser Laboratory National University of Defense TechnologyChangsha 410073China

This paper presents an efficient scheme for single-pixel imaging(SPI)utilizing a phase-controlled fiber laser array and an untrained deep neural network.The fiber lasers are arranged in a compact hexagonal structure and coherently combined to generate illuminating light fields.Through the utilization of high-speed electro-optic modulators in each individual fiber laser module,the randomly modulated fiber laser array enables rapid speckle projection onto the object of interest.Furthermore,the untrained deep neural network is incorporated into the image reconstructing process to enhance the quality of the reconstructed images.Through simulations and experiments,we validate the feasibility of the proposed method and successfully achieve high-quality SPI utilizing the coherent fiber laser array at a sampling ratio of 1.6%.Given its potential for high emitting power and rapid modulation,the SPI scheme based on the fiber laser array holds promise for broad applications in remote sensing and other applicable fields.

关键词： Single-pixel imaging Fiber laser array Deep learning Remote sensing

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Superior efficiency and stability of YbO_(x)-enhanced perovskite solar cells

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Science China Materials 2024年第4期67卷 1356-1358页

作者： Qifeng Zhang guozhong Cao Department of Electrical and Computer Engineering North Dakota State UniversityFargoND 58108-6050USA Department of Materials Science and Engineering University of WashingtonSeattleWA 98195-2120USA

Perovskite solar cells represent a revolutionary class of photovoltaic devices that have gained substantial attention for their exceptional performance and potential to provide an affordable and efficient solution for harnessing solar energy. These cells utilize perovskite-structured materials, typically hybrid organicinorganic lead halide compounds, as the light-absorbing layer.

关键词： energy perovskite stability

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Highly sensitive flexible strain sensor based on the two-dimensional semiconductor tellurium with a negative gauge factor

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Science China(Information Sciences) 2024年第7期67卷 295-304页

作者： Jiarui HE Yusong QU Shengyao CHEN Cong wang Lena DU Xiaoshan DU Yuanyuan ZHENG guozhong ZHAO He TIAN College of Mathematics and Physics Beijing University of Chemical Technology School of Integrated Circuits Tsinghua University Beijing China & The Beijing National Research Center for Information Science and Technology (BNRist)Tsinghua University CAS Center for Excellence in Nanoscience National Center for Nanoscience and Technology &University of Chinese Academy of Sciences Beijing Key Lab of Terahertz Spectroscopy and Imaging Key Lab of Terahertz OptoelectronicsMinistry of Education Department of Physics Capital Normal University

Research on flexible strain sensors has advanced rapidly in recent years, with particular attention being devoted to two-dimensional(2D) semiconductor materials owing to their exceptional mechanical and electrical properties that are conducive to sophisticated sensing performance. However, resistive strain sensors based on 2D semiconductor materials typically exhibit positive gauge factors(GF), while materials for strain sensors with a negative GF remain elusive. We have identified a trend of reduction in the band gap of the emerging 2D semiconductor material tellurium(Te) under strain in simulations reported in past research,and have observed a negative GF in the Te-based strain sensor. In this study, we combined Te with a flexible polyethylene terephthalate(PET) substrate to manufacture a flexible strain sensor with a significantly negative GF. The results of tests revealed that the Te-based strain sensor achieved an impressive maximum sensitivity of-139.7 within a small range of bending-induced strain(< 1%). Furthermore, it exhibited excellent linearity and good cyclic stability, and was successfully applied to monitor limb movements. The work here verifies the significant potential for the use of Te-based strain sensors in next-generation flexible electronics.

关键词： 2D semiconductor materials 2D tellurium flexibleelectronics strain sensors negative gauge factor high sensitivity

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Genetic diversity of RNA viruses infecting invertebrate pests of rice

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Science China(Life Sciences) 2024年第1期67卷 175-187页

作者： Haoran wang Shufen Chao Qing Yan Shu Zhang Guoqing Chen Chonghui Mao Yang Hu Fengquan Yu Shuo wang Liang Lv Baojun Yang Jiachun He Songbai Zhang Liangsheng Zhang Peter Simmonds guozhong Feng State Key Laboratory of Rice Biology and Breeding China National Rice Research InstituteChinese Academy of Agricultural SciencesHangzhou 311400China State Key Laboratory of Agricultural Microbiology College of Life Science and TechnologyHuazhong Agricultural UniversityWuhan 430070China Institute of Plant Protection&Soil Fertilizer Hubei Academy of Agricultural SciencesWuhan 430064China Institute of Plant Protection Guizhou Academy of Agricultural SciencesGuiyang 550000China Institute of Plant Protection Liaoning Academy of Agricultural SciencesShenyang 110161China Sanya Agricultural Technology Extension and Service Centre Sanya 572000China College of Agriculture Yangtze UniversityJingzhou 434000China Fujian Provincial Key Laboratory of Haixia Applied Plant Systems Biology Fujian Agriculture and Forestry UniversityFuzhou 350002China Genomics and Genetic Engineering Laboratory of Ornamental Plants College of Agriculture and BiotechnologyZhejiang UniversityHangzhou 310012China Nuffield Department of Medicine Peter Medawar Building for Pathogen ResearchUniversity of OxfordOxford OX13SYUnited Kingdom

Invertebrate species are a natural reservoir of viral genetic diversity,and invertebrate pests are widely distributed in crop fields.However,information on viruses infecting invertebrate pests of crops is limited.In this report,we describe the deep metatranscriptomic sequencing of 88 invertebrate samples covering all major invertebrate pests in rice fields.We identified 296 new RNA viruses and 13 known RNA viruses.These viruses clustered within 31 families,with many highly divergent viruses constituting potentially new families and genera.Of the identified viruses,13 RNA viruses clustered within the Fiersviridae family of bacteriophages,and 48 RNA viruses clustered within families and genera of mycoviruses.We detected known rice viruses in novel invertebrate hosts at high abundances.Furthermore,some novel RNA viruses have genome structures closely matching to known plant viruses and clustered within genera of several plant virus species.Fortyfive potential insect pathogenic RNA viruses were detected in invertebrate species.Our analysis revealed that host taxonomy plays a major role and geographical location plays an important role in structuring viral diversity.Cross-species transmission of RNA viruses was detected between invertebrate hosts.Newly identified viral genomes showed extensive variation for invertebrate viral families or genera.Together,the large-scale metatranscriptomic analysis greatly expands our understanding of RNA viruses in rice invertebrate species,the results provide valuable information for developing efficient strategies to manage insect pests and virus-mediated crop diseases.

关键词： invertebrate species metatranscriptome viral diversity viral transmission viral genomes

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Superior efficiency and stability of YbO-enhanced perovskite solar cells

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Science China Materials 2024年

作者： Qifeng Zhang guozhong Cao Department of Materials Science and Engineering University of Washington Department of Electrical and Computer Engineering North Dakota State University

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Interfacial engineering of metallic rhodium by thiol modification approach for ambient electrosynthesis of ammonia

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Nano Research 2022年第10期15卷 8826-8835页

作者： Meng Jin Xinyuan Zhang Xian Zhang Hongjian Zhou Miaomiao Han Yunxia Zhang guozhong wang 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 230031China University of Science and Technology of China Hefei 230026China School of Science Huzhou UniversityHuzhou 313000China

Here we report a vapor-phase reaction approach to fabricate rhodium(I)-dodecanethiol complex coated on carbon fiber cloth(Rh(I)-SC_(12)H_(25)/CFC),followed by low-temperature pyrolysis to achieve dodecanethiol modified Rh(Rh@SC_(12)H_(2)5/CFC)for electrocatalytic nitrogen reduction reaction(NRR).The results demonstrate that after pyrolysis for 0.5 h at 150℃,the obtained Rh@SC_(12)H_(2)5/CFC-0.5 exhibits excellent NRR activity with an NH3 yield rate of 121.2±6.6μg∙h^(−1)∙cm^(−2)(or 137.7±7.5μg∙h^(−1)∙mgRh^(−1))and a faradaic efficiency(FE)of 51.6%±3.8%at−0.2 V(vs.RHE)in 0.1 M Na_(2)SO_(4).The theoretical calculations unveil that the adsorption of dodecanethiol on the hollow sites of Rh(111)plane is thermodynamically favorable,effectively regulating the electronic structure and surface wettability of metallic Rh.Importantly,the dodecanethiol modification on Rh(111)obviously decreases the surface H*coverage,thus inhibiting the competitive hydrogen evolution reaction and concurrently reducing the electrocatalytic NRR energy barrier.

关键词： dodecanethiol modification electrocatalysis low temperature pyrolysis nitrogen reduction reaction surface H*coverage

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Fatigue Resistance of RCA Modified Asphalt Based on Dielectric Properties

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Journal of Wuhan University of Technology(Materials Science) 2024年第1期39卷 91-101页

作者：陆佳宝王国忠 HU Jiangsan LIU Zhongning College of Energy and Transportation Engineering Inner Mongolia Agricultural UniversityHohhot 010018China

In order to study the anti-fatigue performance of RCA modified asphalt (RMA),the performance of RMA and 90#matrix asphalt with different modifier content were measured by asphalt penetration,ductility,softening point,Brookfield viscosity,rheological index,infrared spectrum and dielectric constant test.This paper discusses the changes of asphalt basic indexes,fatigue properties and asphalt components based on dielectric properties under different modifier contents,and analyzes the grey correlation degree between components and asphalt pavement performance indexes.The results show that the optimum content of RCA modifier is 16.7%of the asphalt quality according to the penetration,ductility,softening point,Brockfield viscosity,viscosity temperature curve and fatigue life.In the phase angle-strain curve,there is disorder in the latter part of the curve.According to the strain (ε_(d)) corresponding to the disorder point,a new fatigue failure criterion is proposed and proved.Based on the new asphalt fatigue failure criterion,the fatigue prediction model of asphalt mixture is improved,and the fatigue life predicted by the improved fatigue model is compared with the fatigue life obtained by four-point bending fatigue test.The results show that the proposed new asphalt fatigue failure criterion is reasonable,and the fatigue life predicted by the improved asphalt mixture fatigue prediction model is accurate.The research method of classifying asphalt components based on dielectric properties is simple and effective,and the components have a high correlation with the road performance of base asphalt and modified asphalt.

关键词： dielectric properties anti-fatigue performance fatigue failure criterion RCA modified asphalt

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