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Electronic structure engineering of single atomic sites by plasmoninduced hot electrons for highly efficient and selective photocatalysis

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Nano Research 2024年第8期17卷 6960-6967页

作者： Xiaoya Huang Xinyuan Li Akang Chen Hongfei Gu Shouyuan Li Tailei Hou Shuwen Zhu Shuang Yu Yin Song Jiatao Zhang Beijing Key Laboratory of Construction Tailorable advanced Functional Materials and Green Applications MIIT Key Laboratory of Medical Molecule Science and Pharmaceutical EngineeringMOE Key Laboratory of Cluster ScienceSchool of Chemistry and Chemical EngineeringSchool of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China MIIT Key Laboratory of Complex-field Intelligent Exploration School of Optics and PhotonicsBeijing Institute of TechnologyBeijing 100081China

Single atom(SA)catalysts have achieved great success on highly selective heterogeneous catalysis due to their abundant and homogeneous active *** electronic structures of these active sites,restrained by their localized coordination environments,significantly determine their catalytic performances,which are difficult to ***,we investigated the effect of localized surface plasmon resonance(LSPR)on engineering the electronic structures of single atomic ***,core–shell structures consisted of Au core and transition metal SAs loaded N-doped carbon(CN)shell were constructed,namely Au@M-SA/CN(M=Ni,Fe,and Co).It was demonstrated that plasmon-induced hot electrons originated from Au were directionally injected to the M-SAs under visible light irradiation,which significantly changed their electronic structures and meanwhile facilitated improved overall charge separation *** as-prepared Au@Ni-SA/CN exhibited highly efficient and selective photocatalytic CO_(2) reduction to CO performance,which is 20.8,17.5,and 6.9 times those of Au nanoparticles,Au@CN,and Ni-SA/CN,*** spectroscopy analysis and theoretical calculations confirmed that the plasmon enhanced Ni-SA/CN sites featured increased charge density for efficient intermediate activation,contributing to the superb photocatalytic *** work provides a new insight on plasmon and atomic site engineering for efficient and selective catalysis.

关键词： single atom catalysts plasmon enhancement coupling effect photocatalysis CO_(2) reduction

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Bimetallic NiCoP catalysts anchored on phosphorus-doped lignin-based carbon for robust oxygen evolution performance

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Rare Metals 2024年第7期43卷 3084-3095页

作者： Ling-Ying-Zi Xiong Bo-Wen Liu Lei Du Yue-Kuan Zhou Xu-Liang Lin Huan Wang Guangdong Engineering Technology Research Center for Sensing Materials&Devices Guangzhou Key Laboratory of Sensing Materials&DevicesSchool of Chemistry and Chemical EngineeringGuangzhou UniversityGuangzhou 510006China School of Chemical Engineering and light Industry Guangdong University of TechnologyGuangzhou 510006China Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center Jieyang 515200China Sustainable Energy and Environment Thrust Function HubThe Hong Kong University of Science and Technology(Guangzhou)Guangzhou 511400China Division of Emerging Interdisciplinary Areas Department of Mechanical and Aerospace EngineeringThe Hong Kong University of Science and TechnologyHong Kong 999077China State Key Lab of Pulp and Paper Engineering South China University of TechnologyGuangzhou 510640China

Oxygen evolution reaction(OER)catalysts are the key core materials that determine the performance of fuel cells,metal-air batteries,electrolytic water decomposition,and other *** this work,a green lignin-based non-precious metal OER catalyst was prepared by a simple ***,c arboxylated lignin was used to complex Ni and Co in situ,and then they were placed with sodium hypophosphite in the same tube furnace for upstream and downstream high-temperature calcination to construct a lignin carbon-based Ni-Co bimetallic OER catalyst(NiCoP@C).The synthesized catalyst is a porous bimetallic phosphide with a three-dimensional network structure and high-density electrochemical active ***@C exhibited favorable catalytic activity for the oxygen evolution reaction(OER)with overpotential of 280 mV at 10 mA·cm~(-2)and a Tafel slope of 77 mV·dec~(-1).Additionally,it exhibited remarkable durability during *** functional theory(DFT)calculations revealed that by leveraging the distinctive structure of transition metal phosphide nanoparticles incorporated into a reticulated substrate,the NiCoP@C catalyst offered an increased number of active sites for OER catalysis,significantly enhancing its stability during practical *** present study broadens the utilization pathways of biomass to"turn waste into treasure,"aligning the development concept of green sustainable development.

关键词： Oxygen evolution reaction Lignin Carbon-based catalyst Nickel-cobalt bimetal Metal phosphide

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π-Extended giant dimeric acceptor as a third component enables highly efficient ternary organic solar cells with efficiency over 19.2%

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Journal of Energy Chemistry 2024年第8期95卷 263-270,I0006页

作者： Mengran Peng Haotian Wu Liming Wu Jianhua Chen Ruijie Ma Qunping Fan Hua Tan Weiguo Zhu Hongxiang Li Junqiao Ding School of Chemical Science and Technology Yunnan UniversityKunming 650500YunnanChina Department of Electrical and Electronic Engineering Research Institute for Smart Energy(RISE)Guangdong-Hong Kong-Macao(GHM)Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and DevicesThe Hong Kong Polytechnic UniversityKowloonHong Kong 999077China State Key Laboratory for Mechanical Behavior of Materials Xi’an Jiaotong UniversityXi’an 710049ShaanxiChina School of Materials Science and Engineering Jiangsu Engineering Laboratory of Light-Electricity-Heat Energy-Converting Materials and ApplicationsChangzhou UniversityChangzhou 213164JiangsuChina College of Polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065SichuanChina

Ternary strategy with a suitable third component is a successful strategy to improve the photovoltaic performance of organic solar cells(OSCs).Very recently,Y-series based giant molecule acceptors or oligomerized acceptors have emerged as promising materials for achieving highly efficient and stable binary OSCs,while application as third component for ternary OSCs is *** a novelπ-extended giant dimeric acceptor,GDF,is developed based on central Y series core fusion and rigid BDT as linker,and then incorporated into the state-of-the-art PM1:PC6 system to construct ternary *** GDF has a near planar backbone,resulting in increasedπ-conjugation,excellent crystallinity,and good electron transport *** GDF is introduced into the PM1:PC6 system,it ensues in a cascade like the lowest unoccupied molecular orbitals(LUMO)energy level alignment,a complementary absorption band with PM1 and PC6,higher and balanced hole and electron mobility,slightly smaller domain size,and a higher exciton dissociation probability for PM1:PC6:GDF(1:1.1:0.1)blend *** a consequence,the PM1:PC6:GDF(1:1.1:0.1)ternary OSC achieves a champion PCE of 19.22%,with a significantly higher open-circuit voltage and short-circuit current density,compared to 18.45%for the PM1:PC6(1:1.2)binary *** findings show that employing aπ-extended giant dimeric acceptor as a third component significantly improves the photovoltaic performance of ternary OSCs.

关键词： Giant dimeric acceptor Third component Ternary organic solar cells

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Graphene-driving strain engineering to enable strain-free epitaxy of AlN film for deep ultraviolet light-emitting diode

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light(Science & Applications) 2022年第5期11卷 808-819页

作者： Hongliang Chang Zhetong Liu Shenyuan Yang Yaqi Gao Jingyuan Shan Bingyao Liu Jingyu Sun Zhaolong Chen Jianchang Yan Zhiqiang Liu Junxi Wang Peng Gao Jinmin Li Zhongfan Liu Tongbo Wei Research and Development Center for Semiconductor lighting Technology Institute of SemiconductorsChinese Academy of Sciences100083 BeijingChina Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences100049 BeijingChina Center for Nanochemistry(CNC) Beijing Science and Engineering Center for NanocarbonsBeijing National Laboratory for Molecular SciencesCollege of Chemistry and Molecular EngineeringPeking University100871 BeijingChina Electron microscopy Laboratory and International Center for Quantum MaterialsSchool of PhysicsPeking University100871 BeijingChina Beijing graphene institute(BGI) 100095 BeijingChina Academy for advanced Interdisciplinary Studies Interdisciplinary Institute of Light-Element Quantum Materials and Research Center for Light-Element Advanced MaterialsPeking University100871 BeijingChina State Key Laboratory of Superlattices and Microstructures Institute of SemiconductorsChinese Academy of Sciences100083 BeijingChina

The energy-efficient deep ultraviolet(DUV)optoelectronic devices suffer from critical issues associated with the poor quality and large strain of nitride material system caused by the inherent mismatch of *** this work,we have prepared the strain-free AlN film with low dislocation density(DD)by graphene(Gr)-driving strain-pre-store engineering and a unique mechanism of strain-relaxation in quasi-van der Waals(QvdW)epitaxy is *** DD in AlN epilayer with Gr exhibits an anomalous sawtooth-like evolution during the whole epitaxy *** can help to enable the annihilation of the dislocations originated from the interface between AlN and Gr/sapphire by impelling a lateral two-dimensional growth ***,it can induce AlN epilayer to pre-store sufficient tensile strain during the early growth stage and thus compensate the compressive strain caused by ***,the low-strain state of the DUV light-emitting diode(DUV-LED)epitaxial structure is realized on the strain-free AlN template with ***,the DUV-LED with Gr demonstrate 2.1 times enhancement of light output power and a better stability of luminous wavelength compared to that on bare *** in-depth understanding of this work reveals diverse beneficial impacts of Gr on nitride growth and provides a novel strategy of relaxing the vital requirements of hetero-mismatch in conventional heteroepitaxy.

关键词： sapphire diode strain

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Photomediated core modification of diaryl dihydrophenzines through three-component alkylarylation of alkenes toward organocatalyzed ATRP

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Green Synthesis and Catalysis 2024年第1期5卷 35-41页

作者： Yajun Zhang Hao Wang Dandan Jiang Naixian Sun Wei He Lili Zhao Ning Qin Ning Zhu Zheng Fang Kai Guo College of Biotechnology and Pharmaceutical Engineering State Key Laboratory of Materials-Oriented Chemical EngineeringNanjing Tech UniversityNanjing211800China Institute of advanced Synthesis School of Chemistry and Molecular EngineeringNanjing Tech UniversityNanjing211800China Department of Mechanical Engineering The University of SheffieldSheffieldS13JDUnited Kingdom

The design and synthesis of a novel organic photocatalyst(OPC)have attracted broad interest from both the organic chemistry and polymer ***,we presented a visible-light-induced alkylarylation of alkenes strategy for core modification of 5,10-diaryl-5,10-dihydrophenazines(DADHPs)under metal-and additive-free conditions,with the aim to develop powerful photocatalyst for organocatalyzed atom transfer radical polymerization(O-ATRP).Good tolerance for a wide variety of functional groups and affording the corresponding tetrasubstituted products in moderate to good yields were achieved in the batch and flow *** experimental and computational mechanistic study confirmed that DADHPs’radical cations andπ-πstacking interactions played important roles in the alkylarylation of alkenes.A series of the tetrasubstituted DADHPs were directly synthesized from the corresponding noncore-modified phenazines,which were demonstrated to be effective organic photoredox catalysts for *** responsive nature,controlled polymerization manner,and welldefined poly(methyl methacrylate)were achieved via tetrasubstituted DADHPs mediated O-ATRP.

关键词： Photoinduced core modification Diaryl dihydrophenzine O-ATRP

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Comprehensive understanding and rational regulation of microenvironment for gas-involving electrochemical reactions

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Carbon Energy 2023年第7期5卷 70-99页

作者： Qiyang Cheng Mengfan Wang Jiajie Ni Lifang Zhang Yu Cheng Xi Zhou Yufeng Cao Tao Qian Chenglin Yan School of Chemistry and Chemical Engineering Nantong UniversityNantongChina Key Laboratory of core Technology of High Specific Energy Battery and Key Materials for Petroleum and Chemical Industry College of EnergySoochow UniversitySuzhouChina light Industry Institute of Electrochemical Power Sources Soochow UniversitySuzhouChina

Substantial progress has been made in the understanding of gas-involving electrochemical reactions recently for the sake of clean,renewable,and efficient energy ***,the specific influence mechanism of the microenvironment at the reaction interface on the electrocatalytic performance(activity,selectivity,and durability)remains ***,we provide a comprehensive understanding of the interfacial microenvironment of gas-involving electrocatalysis,including carbon dioxide reduction reaction and nitrogen reduction reaction,and classify the factors affecting the reaction thermodynamics and kinetics into gas diffusion,proton supply,and electron *** categorization allows a systematic survey of the literature focusing on electrolyzer-level(optimization of the device,control of the experimental condition,and design of the working electrode),electrolytelevel(increase of gas solubility,regulation of proton supply,and substitution of anodic reaction),and electrocatalyst-level strategies(promotion of gas affinity,adjustment of hydrophobicity,and enhancement of conductivity),aiming to retrieve the correlations between the microenvironment and electrochemical ***,priorities for future studies are suggested to support the comprehensive improvement of next-generation gas-involving electrochemical reactions.

关键词： CO_(2)RR electrocatalysis microenvironment NRR three-phase interface

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Eff-3DPSeg:3D Organ-Level Plant Shoot Segmentation Using Annotation-Efficient Deep Learning

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Plant Phenomics 2023年第3期5卷 626-641页

作者： Liyi Luo Xintong Jiang Yu Yang Eugene Roy Antony Samy Mark Lefsrud Valerio Hoyos-Villegas Shangpeng Sun Bioresource Engineering Department McGill UniversityMontrealQCCanada Key Laboratory of advanced Process Control for light Industry(Ministry of Education) Jiangnan UniversityWuxiJiangsuChina Plant Science Department McGill UniversityMontrealQCCanada

Reliable and automated 3-dimensional(3D)plant shoot segmentation is a core prerequisite for the extraction of plant phenotypic traits at the organ *** deep learning and point clouds can provide effective ways to address the ***,fully supervised deep learning methods require datasets to be point-wise annotated,which is extremely expensive and *** our work,we proposed a novel weakly supervised framework,Eff-3DPSeg,for 3D plant shoot ***,high-resolution point clouds of soybean were reconstructed using a low-cost photogrammetry system,and the Meshlab-based Plant Annotator was developed for plant point cloud ***,a weakly supervised deep learning method was proposed for plant organ *** method contained(a)pretraining a self-supervised network using Viewpoint Bottleneck loss to learn meaningful intrinsic structure representation from the raw point clouds and(b)fine-tuning the pretrained model with about only 0.5%points being annotated to implement plant organ ***,3 phenotypic traits(stem diameter,leaf width,and leaf length)were *** test the generality of the proposed method,the public dataset Pheno4D was included in this *** results showed that the weakly supervised network obtained similar segmentation performance compared with the fully supervised *** method achieved 95.1%,96.6%,95.8%,and 92.2%in the precision,recall,F1 score,and mIoU for stem–leaf segmentation for the soybean dataset and 53%,62.8%,and 70.3%in the AP,AP@25,and AP@50 for leaf instance segmentation for the Pheno4D *** study provides an effective way for characterizing 3D plant architecture,which will become useful for plant breeders to enhance selection *** trained networks are available at https://***/jieyi-one/EFF-3DPSEG.

关键词： Deep Plant weakly

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Eliminating nitrogen chemisorption barrier with single-atom supported yttrium cluster via electronic promoting effect for highly efficient ammonia synthesis

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Nano Research 2023年第2期16卷 2185-2191页

作者： Yuzhuo Jiang Mengfan Wang Sisi Liu Lifang Zhang Siyi Qian Yufeng Cao Yu Cheng Tao Qian Chenglin Yan School of Chemistry and Chemical Engineering Nantong UniversityNantong 226019China Key Laboratory of core Technology of High Specific Energy Battery and Key Materials for Petroleum and Chemical Industry College of EnergySoochow UniversitySuzhou 215006China light Industry Institute of Electrochemical Power Sources Suzhou 215600China

Nitrogen chemisorption is a prerequisite for efficient ammonia synthesis under ambient conditions,but promoting this process remains a significant ***,by loading yttrium clusters onto a single-atom support,an electronic promoting effect is triggered to successfully eliminate the nitrogen chemisorption barrier and achieve highly efficient ammonia *** functional theory calculations reveal that yttrium clusters with abundant electron orbitals can provide considerable electrons and greatly promote electron backdonation to the N2 antibonding orbitals,making the chemisorption process ***,according to the“hot atom”mechanism,the energy released during exothermic N2 chemisorption would benefit subsequent N2 cleavage and hydrogenation,thereby dramatically reducing the energy barrier of the overall *** expected,the proof-of-concept catalyst achieves a prominent NH3 yield rate of 48.1μg·h^(−1)·mg^(−1)at−0.2 V versus the reversible hydrogen electrode,with a Faradaic efficiency of up to 69.7%.This strategy overcomes one of the most serious obstacles for electrochemical ammonia synthesis,and provides a promising method for the development of catalysts with high catalytic activity and selectivity.

关键词： ammonia synthesis yttrium cluster electronic promoting effect rate-determining step nitrogen chemisorption barrier

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Plasmon-enhanced self-powered GaN/ZnTe core/shell nanopillar array photodetector

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Nano Research 2024年第6期17卷 5569-5577页

作者： Jianqi Dong Dongqi Zhang Yi Ma Daotong You Jinping Chen Bin Liu Xingfu Wang Zengliang Shi Chunxiang Xu State Key Laboratory of Digital Medical Engineering School of Biological Science and Medical EngineeringSoutheast UniversityNanjing 210096China Jiangsu Provincial Key Laboratory of advanced Photonic and Electronic Materials National Laboratory of Solid State MicrostructuresSchool of Electronic Science and EngineeringNanjing UniversityNanjing 210093China Institute of Photonics Technology Jinan UniversityGuangzhou 510632China Guangdong Engineering Research Center of Optoelectronic Functional Materials and Devices Institute of SemiconductorsSouth China Normal UniversityGuangzhou 510631China

Nanostructure photodetectors,as the core component of optoelectronic devices,are mainly focused on the precise preparation of mixed-component nano-heterostructures and the realization of zero power consumption ***,we successfully fabricated n-GaN/p-ZnTe core/shell nanopillar array and realized self-power ultraviolet/violet *** radial heterojunction nanodevice reveals high light-dark current ratio of 104 at 0 V bias,indicating effective carriers’*** more,by integrating plasmonic effect,the responsivity and detectivity of the Au nanoparticles decorated device are increased from 3.85 to 148.83 mA/W and 4.45×1011 to 2.33×1012 Jones under 325 nm UV light *** the rise and the fall time are decreased 1.3 times and 6.8 times under 520 nm visible light irradiation at 0 V *** high photocurrent gain is derived from that the oscillating high-energy hot electrons in Au nanoparticles spontaneously inject into the ZnTe conduction band to involve the photodetection *** work presents an effective route to prepare high-performance self-power photodetector and provides a promising blueprint to realize different functional photoelectronic devices based on core/shell nanostructure.

关键词： GaN/ZnTe core/shell nanopillar array self-power ultraviolet/visible photodetector plasmonic effect

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advanced In Situ Characterization Techniques for Direct Observation of Gas-Involved Electrochemical Reactions

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Energy & Environmental Materials 2023年第6期6卷 73-112页

作者： Yanzheng He Sisi Liu Mengfan Wang Qiyang Cheng Haoqing Ji Tao Qian Chenglin Yan Key Laboratory of core Technology of High Specific Energy Battery and Key Materials for Petroleum and Chemical Industry College of EnergySoochow UniversitySuzhou 215006China School of Chemistry and Chemical Engineering Nantong UniversityNantong 226019China light Industry Institute of Electrochemical Power Sources Suzhou 215600China

Gas-involved electrochemical reactions provide feasible solutions to the worldwide energy crisis and environmental *** has been recognized that various elements of the reaction system,including catalysts,intermediates,and products,will undergo real-time variations during the reaction process,which are of significant meaning to the in-depth understanding of reaction mechanisms,material structure,and active *** judicious tools for real-time monitoring of the changes in these complex elements,in situ techniques have been exposed to the spotlight in recent *** review aims to highlight significant progress of various advanced in situ characterization techniques,such as in situ X-ray based technologies,in situ spectrum technologies,and in situ scanning probe technologies,that enhance our understanding of heterogeneous electrocatalytic carbon dioxide reduction reaction,nitrogen reduction reaction,and hydrogen evolution *** provide a summary of recent advances in the development and applications of these in situ characterization techniques,from the working principle and detection modes to detailed applications in different reactions,along with key questions that need to be ***,in view of the unique application and limitation of different in situ characterization techniques,we conclude by putting forward some insights and perspectives on the development direction and emerging combinations in the future.

关键词： carbon dioxide reduction reaction gas-involved electrochemical reactions hydrogen evolution reaction in situ characterizations nitrogen reduction reaction

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