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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

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

Suppression of Co(Ⅱ)ion deposition and hazards:Regulation of SEI film composition and structure

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Journal of Energy Chemistry 2024年第2期89卷 259-265,I0007页

作者： Jiaqi Zhan Mingzhu Liu Yutian Xie Jiarong He Hebing Zhou Lidan Xing Weishan Li National and Local joint Engineering research center of MPTES in High Energy and Safety LIBs Engineering Research Center of MTEES(Ministry of Education)Research Center of BMET(Guangdong Province)Key Lab.of ETESPG(GHEI)Innovative Platform for ITBMD(Guangzhou Municipality)School of ChemistrySouth China Normal UniversityGuangzhou 510006GuangdongChina

Despite the presence of Li F components in the solid electrolyte interphase(SEI)formed on the graphite anode surface by conventional electrolyte,these Li F components primarily exist in an amorphous state,rendering them incapable of effectively inhibiting the exchange reaction between lithium ions and transition metal ions in the ***,nearly all lithium ions within the SEI film are replaced by transition metal ions,resulting in an increase in interphacial impedance and a decrease in ***,we demonstrate that the SEI film,constructed by fluoroethylene carbonate(FEC)additive rich in crystalline Li F,effectively inhibits the undesired Li^(+)/Co^(2+)ion exchange reaction,thereby suppressing the deposition of cobalt compounds and metallic ***,the deposited cobalt compounds exhibit enhanced structural stability and reduced catalytic activity with minimal impact on the interphacial stability of the graphite *** findings reveal the crucial influence of SEI film composition and structure on the deposition and hazards associated with transition metal ions,providing valuable guidance for designing next-generation electrolytes.

关键词： Lithium-ion batteries Transition metal ions SEI film Composition and structure

Microstructural evolution and deformation behavior of friction stir welded twin-induced plasticity steel

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Journal of Materials Science & Technology 2024年第2期169卷 68-81页

作者： Ke Qiao Kuaishe Wang Jia Wang Zhengyang Hao Yating Xiang Peng Han Jun Cai Qi Yang Wen Wang School of Metallurgical Engineering National and Local Joint Engineering Research Center for Functional Materials ProcessingXi’an University of Architecture and TechnologyXi’an 710055China Shanghai research Institute of Materials Shanghai 200437China

The weldability of twin-induced plasticity(TWIP)steel with ultra-high strength via friction stir welding(FSW)technique was investigated,and microstructural evolution and deformation behavior of whole and micro-zones of FSW TWIP joint were studied for the first *** results showed that the content of recrystallized grains in the stir zone(SZ)increased from 10.5%of basal material(BM)to 14.2%,and that of heat affected zone(HAZ)increased to 78.6%.The percentage of annealing twins decreased from 26.8%in BM to 11%in SZ,while increased to 35%in *** with the BM,the ultimate tensile strength and yield strength of the FSW joint increased to 1036 and 550 MPa,respectively,reaching 106.7%and 110.9%of BM,*** elongation of the entire joint was 50.5%,which was lower than that of BM due to the nonuniform deformation during the tensile *** engineering strain was mainly concentrated in BM and SZ and transferred to each other during the tensile test,while the engineering strain in HAZ was always the ***,the tensile fracture occurred in the *** order of ultimate tensile strength of micro-zones in the FSW joint was as follows:HAZ>BM≈*** order of yield strength was as follows:HAZ>BM>SZ.

关键词： Twin-induced plasticity steel Friction stir welding Microstructure Mechanical property Deformation behavior

Engineering the Interface Between Au Nanoparticles and CoO-Ov to Enhance the Catalytic Performance of 5-Hydroxymethylfurfural(HMF)to 2,5-Dimethylfuran(DMF)

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Chemical research in Chinese Universities 2024年第1期40卷 47-54页

作者： XIANG Shuang GUO Yong LIU Xiaohui WANG Yanqin Key Laboratory for Advanced Materials and joint International research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterResearch Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237P.R.China

The interface between Au and support has attracted extensive interest because of its unique catalytic ability for hydrogen activation in catalytic hydrogenation/hydrogenolysis ***,we create the Au-CoO-OV interface in the 1.0%Au/Co3O4-Rod-250 catalyst,which could dissociate H2 via the heterolytic way to yield rich hydride species and achieve excellent catalytic performance in the hydrogenolysis of biomass-derived 5-hydroxymethylfurfural(HMF)to 2,5-dimethylfuran(DMF).The XRD and HRTEM analyses show that Au nanoparticles are uniformly dispersed on CoO-OV surface and in situ DRIFTS spectra show the enhancement of heterolytic dissociation of hydrogen(signals of Au-D and O-D vibration)compared with bare CoO(Co3O4-Rod-250).This work provides insights for fabricating highly active Au-support catalysts for catalytic hydrogenation/hydrogenolysis reactions.

关键词： Au-CoO-OV interface Hydride species Heterolytic dissociation 5-Hydroxymethylfurfural(HMF) 2 5-Dimethylfuran(DMF)

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

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Nickel-Catalyzed Regiodivergent Acylzincation of Styrenes with Organozincs and CO

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Chinese Journal of Chemistry 2024年第6期42卷 599-604页

作者： Chenglong Wang Ning Liu Xianqing Wu Jingping Qu Yifeng Chen 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 TechnologyShanghai200237 China Dedicated to the Special Issue of C1 Chemistry.

Transition metal-catalyzed carbometallation of unsaturated hydrocarbons constitutes one of the most efficient synthetic methodologies for the construction of C—C ***,the incorporation of organometallic reagent with the CO gas as a nucleophilic acyl synthon could enable the acylmetallation reaction,which greatly increases the horizon of carbometallation ***,we report a nickel-catalyzed regiodivergent acylzincation of o-cyano cinnamate ester and o-cyano styrene,in which the cyano moiety intramolecularly captures zinc intermediates to trigger the tandem cyclization *** protocol features mild conditions,broad substrate scope and excellent functional group tolerance,thus affording a diverse array of highly functionalized carbocyclic compounds.

关键词： Carbonylation Carbometallation Styrene Nickel Cyclization