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Developing silicon-based photocathodes for CO_(2) conversion

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Science China Chemistry 2024年第6期67卷 1904-1921页

作者： Weijie Zhuang Miao Kan Tao Meng Jinlong Zhang Key Laboratory for Advanced Materials and joint International research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai200237China Shanghai Engineering research center for Multimedia Environmental Catalysis and Resource Utilization East China University of Science and TechnologyShanghai200237China

Photoelectrochemical(PEC)conversion of CO_(2) presents a promising avenue for solar-driven chemical fuel production,with silicon emerging as a cost-effective and high-light-absorbing material pivotal to this *** at exploring opportunities for industrializing PEC CO_(2) reduction(PEC-CO_(2)R)by minimizing reaction energy consumption,enhancing reaction efficiency and selectivity,this review summarizes recent advancements in developing Si-based photocathodes for PEC-CO_(2)*** outlines the fundamental principles,advantages,and limitations of Si photocathodes with key performance *** on this understanding,the strategies to enhance the performance of the PEC-CO_(2)R system,including light absorption,charge separation,and catalytic reactions are categorized as the interfacial modification,active site decoration,and protective layer *** design ideas of this advantageous three-layer structure in promoting the efficiency,stability,and selectivity have been ***,this review scrutinizes the influence of the photocathodic chemical *** review consolidates the mechanism insights and notable breakthroughs of various fuel generation processes within Si-based PEC-CO_(2)R *** this wealth of information offers an up-to-date perspective on the dynamic developments in silicon-based PEC-CO_(2) conversion and underscores the promising pathways toward the sustainable fuel synthesis from pollutant CO_(2).

关键词： photoelectrochemistry solar fuels silicon photocathodes carbon dioxide reduction microenvironment

Photoelectrochemical seawater oxidation with metal oxide materials:Challenges and opportunities

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Journal of Energy Chemistry 2024年第10期97卷 767-782,I0016页

作者： Miao Kan Hangyu Hu Weijie Zhuang Meng Tao Shiqun Wu Jinlong Zhang Key Laboratory for Advanced Materials and joint International research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China Shanghai Engineering research center for Multimedia Environmental Catalysis and Resource Utilization East China University of Science and TechnologyShanghai 200237 China

Photocatalytic water oxidation is a crucial counter-electrode reaction in the process of photoelectrochemical energy *** its importance,challenges remain in effectively and sustainably converting water to oxygen,particularly with readily available and inexpensive electrolyte solutions such as *** metal oxide materials have demonstrated their advantages in promoting efficiency by reducing overpotential and improving light utilization,stability remains limited by corrosion in multicomponent *** this paper,we reviewed the relationship between four basic concepts including photoelectrochemistry,metal oxide,water oxidation and seawater to better understand the challenges and opportunities in photoelectrochemical(PEC)seawater *** overcome these challenges,the advances in material design,interfacial modification,local environment control and reactor design have been further reviewed to benefit the industrial PEC seawater ***,we demonstrate engineered layered metal oxide electrodes and cell structures that enable powerful and stable seawater *** also outline and advise on the future direction in this area.

关键词： Photoelectrochemistry Anode Water oxidation Metal oxide Seawater Stability

GOES-16 ABI Brightness Temperature Observations Capturing Vortex Rossby Wave Signals during Rapid Intensification of Hurricane Irma(2017)

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Journal of Meteorological research 2024年第4期38卷 768-783页

作者： Yanyang HU Xiaolei ZOU joint center of Data Assimilation for research and Application Nanjing University of Information Science&TechnologyNanjing 210044

Geostationary Operational Environmental Satellite-16(GOES-16) Advanced Baseline Imager(ABI) observations of brightness temperature(TB) are used to examine the temporal evolutions of convection-affected structures of Hurricane Irma(2017) during its rapid intensification(RI) period from 0600 to 1800 UTC 4 September *** ABI observations reveal that both an elliptical eye and a spiral rainband that originated from Irma's eyewall obviously exhibit wavenumber-2 TB *** elliptical eye underwent a counterclockwise rotation at a mean speed of a wavenumber-2 vortex Rossby edge wave from 0815 to 1005 UTC 4 *** the following about 2 hours(1025–1255 UTC 4 September),an inner spiral rainband originated from the eyewall and propagated at a phase speed that approximates the vortex Rossby wave(VRW) phase speed calculated from the aircraft reconnaissance *** the RI period of Irma,ABI TB observations show an on–off occurrence of low TB intrusions into the eye,accompanying a phase lock of eyewall TB asymmetries of wavenumbers 1 and 2 and an outward propagation of VRW-like inner spiral rainbands from the *** phase lock leads to an energy growth of Irma's eyewall *** the eye remained clear from 1415 to 1725 UTC 4 September,an inner spiral rainband that originated from a large convective area also had a VRW-like outward propagation,which is probably due to a vertical tilt of *** study suggests a potential link between convection sensitive GOES imager observations and hurricane dynamics.

关键词： Geostationary Operational Environmental Satellite(GOES)imager brightness temperature(TB) hurricane vortex Rossby wave(VRW)

Chemotactic nanomotor for multimodal combined therapy of glioblastoma

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Science China Chemistry 2024年第4期67卷 1277-1288页

作者： Ting Li Lin Chen Yunxin Xue Xiangyu Xiao Wenjun Dai Kaiyuan Tan Tiantian Chen Yingfang Tao Chun Mao Jian Shen Mimi Wan National and Local joint Engineering research center of Biomedical Functional Materials School of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China

Glioblastoma(GBM) is the most aggressive malignant brain tumor. Due to the infiltration and heterogeneity of GBM, the obstruction of the blood-brain barrier(BBB) and the unique immunosuppressive mechanism, it is hard to achieve significant effects of GBM treatment. Here, a kind of chemotactic nanomotor that loaded with glucose oxidase(GOx) and carboxylated cisplatin(Pt(IV)) prodrug on the L-arginine-derived polymer is proposed. The nanomotors are driven by catalysis of glucose decomposition and the positive chemotaxis towards the GBM microenvironment where inducible nitric oxide synthase and reactive oxygen species are highly expressed. This facilitates the BBB crossing and GBM targeting of the nanomotors. In addition, the released nitric oxide(NO) during propulsion as well as the loaded GOx and Pt(IV) can exert combined NO/starvation/chemotherapy. Meanwhile, it is able to induce and enhance the immune response through multiple pathways, thus better coping with the complexities of GBM treatment.

关键词： chemotaxis combined therapy glioblastoma nanomotors

PdCu alloy anchored defective titania for photocatalytic conversion of carbon dioxide into methane with 100% selectivity

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Journal of Energy Chemistry 2024年第4期91卷 254-265页

作者： Lina Zhang Sajjad Hussain Qiuye Li Jianjun Yang National&Local joint Engineering research center for Applied Technology of Hybrid Nanomaterials Henan UniversityKaifeng 475004HenanChina

The photoreduction of CO_(2)into CH_(4)with simultaneous high activity and selectivity is a promising strategy to increase energy supply and alleviate global ***,the absence of the active sites that is responsible for the adsorption and activation of CO_(2)and the generation of CO and H2via side reactions often lead to poor efficiency and low selectivity of the ***,Cu,Pd,and PdCu metal clusters cocatalyst-anchored defective TiO_(2)nanotubes(Cu/TiO_(2)-SBO,Pd/TiO_(2)-SBO,and Pd1Cu1/TiO_(2)-SBO)were designed via a simple solution impregnation reduction and applied for photocatalytic conversion of CO_(2)to CH_(4).The Pd1Cu1/TiO_(2)-SBO photocatalyst exhibits excellent catalytic performance among the other catalysts for photoreduction of CO_(2)into CH_(4).More interestingly,the product selectivity of CH_(4)reaches up to 100%with a rate of 25μmol g^(-1)h^(-1).In-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and density functional theory(DFT)simulations indicate that the main reasons for the high selectivity of CH_(4)are attributed to the PdCu alloy and oxygen vacancies,which jointly enhance the photoinduced carrier separation and lower energy barriers of key ***,due to the tunable d-band center of the Cu site in the PdCu alloy,the generated intermediates can be well prevented from poisoning and promoted to participate in further ***,the current study will provide insight into the development of new,highly selective photocatalysts for the visible light-catalytic reduction of CO_(2)into CH_(4).

关键词： PdCu alloy Defective TiO_(2) Photoreduction of CO_(2) Photocatalytic mechanism

Molecule configurations modulate packing array and charge transfer in cocrystal engineering

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Science China Chemistry 2024年第2期67卷 512-516页

作者： Shenglong An Mengyuan Qiao Xin Jin Xuanying Chen Jianhua Su Lifang Guo Zhiyun Zhang Key Laboratory for Advanced Materials and joint International research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CentreFrontiers Science Center for Materiobiology and Dynamic ChemistryEast China University of Science&TechnologyShanghai200237China

Organic cocrystal as an emerging assembly strategy has received increasing attention in constructing multiple functional materials,through continually screening suitable constituent monomers or changing their stoichiometry ***,the role of molecule configuration in the cocrystal field is rarely explored despite the fascinating potential in regulating the packing *** this study,the N,N′-diphenyl-5,10-dihydrophenazine derivatives(DPPs) with the flexible scaffold and different methyl substitutions are selected as the donors bearing various molecular *** a simple collaborative way,a series of cocrystals based on DPPs and OFN(octafluoronaphthalene) are fabricated,exhibiting two self-adaptive molecular stacking arrays.X-ray crystallographic analysis and theoretical calculation unveil their different π···π interactions and charge transfer characters,leading to the significant emission redshift up to 125 nm compared with individual *** a result,controllable molecule stacking structure,tunable emission,and charge transfer properties can be *** study provides a new perspective to reveal the structure-property relationships at the molecular level by controlling the molecule configuration in cocrystal engineering,contributing to the development of cocrystal theoretical physics and organic functional materials.

关键词： cocrystals molecular configuration self-adaptive packing mode charge transfer

Understanding adversarial attacks on observations in deep reinforcement learning

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Science China(Information Sciences) 2024年第5期67卷 69-83页

作者： You QIAOBEN Chengyang YING Xinning ZHOU Hang SU Jun ZHU Bo ZHANG Department of Computer Science and Technology Beijing National Research Center for Information Science and Technology Tsinghua-Bosch Joint Center for Machine Learning Institute for Artificial Intelligence Tsinghua University Peng Cheng Laboratory

Deep reinforcement learning models are vulnerable to adversarial attacks that can decrease the cumulative expected reward of a victim by manipulating its observations. Despite the efficiency of previous optimization-based methods for generating adversarial noise in supervised learning, such methods might not achieve the lowest cumulative reward since they do not generally explore the environmental ***, a framework is provided to better understand the existing methods by reformulating the problem of adversarial attacks on reinforcement learning in the function space. The reformulation approach adopted herein generates an optimal adversary in the function space of targeted attacks, repelling them via a generic two-stage framework. In the first stage, a deceptive policy is trained by hacking the environment and discovering a set of trajectories routing to the lowest reward or the worst-case performance. Next, the adversary misleads the victim to imitate the deceptive policy by perturbing the observations. Compared to existing approaches, it is theoretically shown that our adversary is strong under an appropriate noise level. Extensive experiments demonstrate the superiority of the proposed method in terms of efficiency and effectiveness, achieving state-of-the-art performance in both Atari and MuJoCo environments.

关键词： deep learning reinforcement learning adversarial robustness adversarial attack

Photoinduced Bending and Curling Motions in Molecular Microcrystals of Naphthyl Meldrum’s Acid Derivative Based on E-to-Z Photoisomerization

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Chemical research in Chinese Universities 2024年第5期40卷 907-913页

作者： ZHANG Xiaowen XU Tianyi ZHANG Chenchen TONG Fei Key Laboratory for Advanced Materials and joint International research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistrySchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai200237P.R.China

Dynamic photoresponsive molecular crystals are promising candidates for making intelligent devices and materials in the ***,we synthesized a new photoactive molecule(E)-2,2-dimethyl-5-[3-(naphthalen-1-yl)allylide]-1,3-dioxane-4,6-dione[(E)-DNADD]that undergoes an E-to-Z photoisomerization in both liquid solution and solids when exposed to visible light(405 nm).Compared to the bulk crystals,the photoresponsive behavior in microcrystals was profoundly *** crystalline(E)-DNADD microplate crystals exhibit robust motions,including bending,curling,and coiling under light *** photoproduct conversion of the photochemical reaction in the microplate is no more than 20%,while the large bending curvature of the coiled illuminated samples was estimated at approximately 150–300 mm−1,comparable to some photoactive *** results indicate that shrinking crystal dimensions can boost the photoresponses in molecular crystals and provide a facile strategy for developing dynamic molecular crystals at the microscopic scale.

关键词： Photochemistry Molecular crystal E-to-Z photoisomerization Photoinduced motion

Advancing brain-inspired computing with hybrid neural networks

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National Science Review 2024年第5期11卷 56-71页

作者： Faqiang Liu Hao Zheng Songchen Ma Weihao Zhang Xue Liu Yansong Chua Luping Shi Rong Zhao center for Brain-Inspired Computing research Optical Memory National Engineering Research CenterTsinghua University-China Electronics Technology HIK Group Co.Joint Research Center for Brain-inspired ComputingIDGMc Govern Institute for Brain Research Department of Precision Instrument Tsinghua University Neuromorphic Computing Laboratory China Nanhu Academy of Electronics and Information Technology

Brain-inspired computing, drawing inspiration from the fundamental structure and information-processing mechanisms of the human brain, has gained significant momentum in recent years. It has emerged as a research paradigm centered on brain–computer dual-driven and multi-network integration. One noteworthy instance of this paradigm is the hybrid neural network(HNN), which integrates computer-science-oriented artificial neural networks(ANNs) with neuroscience-oriented spiking neural networks(SNNs). HNNs exhibit distinct advantages in various intelligent tasks, including perception, cognition and learning. This paper presents a comprehensive review of HNNs with an emphasis on their origin, concepts, biological perspective, construction framework and supporting systems. Furthermore, insights and suggestions for potential research directions are provided aiming to propel the advancement of the HNN paradigm.

关键词： brain-inspired computing hybrid neural network dual-brain driven multi-network integration neuromorphic system