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Self-optimized H-adsorption affinity of CuRu alloy cocatalysts towards efficient photocatalytic H_(2)evolution

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Journal of Materials Science & Technology 2024年第7期174卷 168-175页

作者： Meiya wang Ping wang Xuefei wang Feng Chen Huogen Yu School of Chemistry Chemical Engineering and Life Sciencesand School of Materials Science and EngineeringWuhan University of TechnologyWuhan 430070China Laboratory of Solar Fuel Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan 430078China

In addition to the electron transfer,the appropriate H-adsorption affinity of active centers on the metal cocatalyst surface is quite important for high hydrogen-production activity of cocatalyst-modified *** typical Cu and Ru metal cocatalysts clearly exhibit a weak Cu-H bond and a strong Ru-H bond,respectively,resulting in limited activity for photocatalytic H_(2)*** this work,an ingenious strategy of self-optimized H-adsorption affinity in CuRu alloy cocatalyst is developed to simultaneously reinforce the Cu-H bond and weaken the Ru-H bond by the intrinsic electron transfer from Cu to Ru *** CuRu alloy nanoparticles(2-3 nm)were deposited on the TiO_(2)surface to prepare CuRu/TiO_(2)through a one-step photoreduction *** tests exhibited that the highest H_(2)-production rate of CuRu/TiO_(2)photocatalyst reached up to 5.316 mmol h^(-1)g^(-1),which was 24.80,1.86,and 2.60 times higher than that of the TiO_(2),Cu/TiO_(2),and Ru/TiO_(2),*** on the characterization results and theoretical calculations,the CuRu alloy cocatalyst exhibits excellent self-optimized H-adsorption affinity via the spontaneous electron transfer from Cu to Ru atom,which can greatly accelerate the photocatalytic H_(2)-production rate of TiO_(2).This work provides a feasible idea for the self-optimized H-adsorption affinity of metal active sites in the photocatalytic H_(2)-generation field.

关键词： TiO_(2) CuRu alloy Cocatalyst Self-optimized H-adsorption affinity Photocatalytic H_(2)generation

Steel-refractory reactions in lanthanum-,cerium-,and ytrium-added steels

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Journal of Iron and Steel Research International 2024年第6期31卷 1473-1485页

作者： Jian Kang Hong-po wang Yu wang College of Materials Science and Engineering Chongqing UniversityChongqing 400044China The State Key Laboratory of Mechanical Transmissions Chongqing UniversityChongqing 400044China

A systematic experimental study was conducted on the similarities and differences in the reactions between commonly used rare earth elements(REEs)and frequently used refractories in the steelmaking *** results indicate that the reaction behaviors of La,Ce,and Y with MgO,Al_(2)O_(3),and MgO·Al_(2)O_(3) crucibles differed *** consumption rates of La,Ce,and Y in the molten steel were in descending order of La>Ce>Y for smelting with all three kinds of *** the REEs reacted with the crucible,the contents of Mg and Al showed a trend of first increasing and then *** laboratory-scale smelting conditions,the reactions related to REEs were dominated by steel-crucible reactions,and the contact area between the unit mass of molten steel and refractory materials mainly determined the consumption rates of ***-and Ce-crucible reactions generated loose and porous reaction interfaces;however,Y-crucible reactions generated a dense Y_(2)O_(3) layer,dramatically suppressing the consumption rate of *** calculation indicated that the reactions between rare earth and different refractory materials were first-order *** crucible materials significantly affected the product type and morphology of the steel-crucible reaction interfaces,thereby influencing the consumption rate of *** reactions between REEs and refractories must be seriously considered,especially for small-scale smelting.

关键词： Rare earth Inclusion Refractory Thermodynamics Dynamics

A synergetic strategy of NIR-Ⅱ squaraine dyes with ultrahigh photothermal conversion efficiency for photothermal therapy

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Science China Chemistry 2024年第2期67卷 612-621页

作者： Yigang wang Guomin Xia Junhui wang Mingda wang Weihan Guo Manman Tan Leilei Si Yang Yang Hua wang Hongming wang Institute for Advanced Study and School of Chemistry and Chemical Engineering Nanchang UniversityNanchang330031China State Key Laboratory of Molecular Reaction Dynamics and Dynamics Research Center for Energy and Environmental Materials Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian116023China The Second Affiliated Hospital of Nanchang University Nanchang330031China

Recent research on photothermal therapy(PTT) has sparked significant interest in the development of new organic photothermal agents(PTAs),ranging from single-molecule to aggregated ***,controlling aggregation pathways for PTAs with ultrahigh photothermal conversion efficiency(PCE) remains a major ***,a two-pronged approach utilizing “Haggregation” and “intramolecular motion” was employed to enhance the PCE of an acceptor-substituted squaraine dye(NSQs).The C2vmolecular symmetry of the NSQs,which possess a ground state dipole moment(μg),promotes H-dimeric aggregates through dipole-dipole *** triphenylethylene or diphenylamine groups were added to this H-dimeric *** was done to enhance intramolecular motions for heat generation and also to extend conjugation,which redshifted the optical absorption and balanced the blue-shift induced by *** this technique,an organic PTA with NIR-II absorption was developed,and its nanoparticle achieved a remarkable PCE of 86.3% under 1,064 nm laser *** transient absorption spectroscopy and quantum mechanical calculations demonstrated the accelerated internal conversion process in NIR-II PTAs for rapid heat *** NSQs nanoparticles exhibit superior photothermal therapeutic properties for in vivo photoacoustic imaging-guided PTT,demonstrating the potential of bottom-up design to enable synergistic engineering strategies towards efficient phototheranostic agents.

关键词： squaraine dyes second near-infrared window H-aggregation intramolecular motion photothermal therapy

Surface Deposition of Ni(OH)_(2) and Lattice Distortion Induce the Electrochromic Performance Decay of NiO Films in Alkaline Electrolyte

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Energy & Environmental Materials 2024年第3期7卷 257-267页

作者： Kejun Xu Liuying wang Chaoqun Ge Long wang Bin wang Zhuo wang Chuanwei Zhang Gu Liu Xi'an Research Institute of High Technology Xi'an 710025China School of Material Science and Engineering Zhengzhou UniversityZhengzhou 450001China School of Mechanical Engineering Xi'an University of Science and TechnologyXi'an 710054China

NiO,an anodic electrochromic material,has applications in energy-saving windows,intelligent displays,and military ***,its electrochromic mechanism and reasons for its performance degradation in alkaline aqueous electrolytes are complex and poorly understood,making it challenging to improve NiO thin *** studied the phases and electrochemical characteristics of NiO films in different states(initial,colored,bleached and after 8000 cycles)and identified three main reasons for performance ***,Ni(OH)_(2)is generated during electrochromic cycling and deposited on the NiO film surface,gradually yielding a NiO@Ni(OH)_(2)core-shell structure,isolating the internal NiO film from the electrolyte,and preventing ion ***,the core-shell structure causes the mode of electrical conduction to change from first-to second-order conduction,reducing the efficiency of ion transfer to the surface Ni(OH)_(2)***,Ni(OH)_(2)and NiOOH,which have similar crystal structures but different b-axis lattice parameters,are formed during electrochromic cycling,and large volume changes in the unit cell reduce the structural stability of the thin ***,we clarified the mechanism of electrochromic performance degradation of NiO films in alkaline aqueous electrolytes and provide a route to activation of NiO films,which will promote the development of electrochromic technology.

关键词： alkaline electrolyte electrochromism NiO film performance attenuation mechanism

Time-sensitive prediction of NO_(2) concentration in China using an ensemble machine learning model from multi-source data

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Journal of Environmental Sciences 2024年第3期137卷 30-40页

作者： Chenliang Tao Man Jia Guoqiang wang Yuqiang Zhang Qingzhu Zhang Xianfeng wang Qiao wang Wenxing wang Big Data Research Center for Ecology and Environment Environment Research InstituteShandong UniversityQingdao 266237China Shandong Provincial Eco-environment Monitoring Center Jinan 250101China

Nitrogen dioxide(NO_(2))poses a critical potential risk to environmental quality and public health.A reliable machine learning(ML)forecasting framework will be useful to provide valuable information to support government *** on the data from1609 air quality monitors across China from 2014-2020,this study designed an ensemble ML model by integrating multiple types of spatial-temporal variables and three sub-models for time-sensitive prediction over a wide *** ensemble ML model incorporates a residual connection to the gated recurrent unit(GRU)network and adopts the advantage of Transformer,extreme gradient boosting(XGBoost)and GRU with residual connection network,resulting in a 4.1%±1.0%lower root mean square error over XGBoost for the test *** ensemble model shows great prediction performance,with coefficient of determination of 0.91,0.86,and 0.77 for 1-hr,3-hr,and 24-hr averages for the test results,*** particular,this model has achieved excellent performance with low spatial uncertainty in Central,East,and North China,the major site-dense *** the interpretability analysis based on the Shapley value for different temporal resolutions,we found that the contribution of atmospheric chemical processes is more important for hourly predictions compared with the daily scale predictions,while the impact of meteorological conditions would be ever-prominent for the *** with existing models for different spatiotemporal scales,the present model can be implemented at any air quality monitoring station across China to facilitate achieving rapid and dependable forecast of NO_(2),which will help developing effective control policies.

关键词： Air quality prediction Deep learning Ensemble method Nitrogen dioxide Spatiotemporal covariates

Assessing the dynamics of O2 desorption from cobalt phthalocyanine by in situ electrochemical scanning tunneling microscopy

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Journal of Energy Chemistry 2024年第11期98卷 144-148页

作者： Yu-Qi wang Yue Feng Xiang wang Dong wang CAS Key Laboratory of Molecular Nanostructure and Nanotechnology CAS Research/Education Center for Excellence in Molecular Sciences Beijing National Laboratory for Molecular Science (BNLMS) Institute of Chemistry Chinese Academy of Sciences University of Chinese Academy of Sciences

We report here the in situ electrochemical scanning tunneling microscopy（ECSTM） study of cobalt phthalocyanine（CoPc）-catalyzed O2evolution reaction（OER） and the dynamics of *** self-assembled CoPc monolayer is fabricated on Au（111） substrate and resolved by ECSTM in 0.1 M KOH *** OH-adsorption on CoPc prior to OER is observed in ECSTM *** OER,the generated O2adsorbed on Co Pc is observed in the CoPc *** step experiment is employed to monitor the desorption of OER-generated O2from CoPc,which results in the decreasing surface coverage of CoPc-O2with *** rate constant of O2desorption is evaluated through data *** insights into the dynamics of Co-O2dissociation at the molecular level via in situ imaging help understand the role of Co-O2in oxygen reduction reaction（ORR） and OER.

关键词： Cobalt phthalocyanine Electrochemical scanning tunneling microscopy Oxygen evolution reaction

Recent advances in solving Li_(2)CO_(3) problems in garnet-based solid-state battery: A systematic review(2020-2023)

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Journal of Energy Chemistry 2024年第3期90卷 58-76,I0004页

作者： Shaoxiong Han Ziqi wang Yue Ma Yanlan Zhang Yongzhen wang Xiaomin wang College of Materials Science and Engineering Taiyuan University of TechnologyTaiyuan 030024ShanxiChina Shanxi Joint Laboratory of Coal based Solid Waste Resource Utilization and Green Ecological Development Taiyuan 030024ShanxiChina

Garnet solid electrolytes are one of the most promising electrolytes for solid-state ***,Li_(2)CO_(3) is a critical issue that hinders the practical application of garnet-based solid-state lithium-ion *** are two sources of Li_(2)CO_(3) *** main one is the aging of garnet electrolytes in the *** electrolytes can react with H_(2)O and CO_(2) in the air to form Li_(2)CO_(3),which reduces ion conductivity,increases electrode/garnet electrolyte interface resistance,and deteriorates the electrochemical performance of the *** strategies,such as elemental doping,grain boundary manipulation,and interface engineering,have been suggested to address these *** other is the passivation layer(Li_(2)CO_(3),Li_3N,LiOH,Li_(2)O) formed on the surface of the lithium foil after long-term storage,which is ignored by most *** better understand the current strategies and future trends to address the Li_(2)CO_(3) problem,this perspective provides a systematic review of journals published in this field from 2020-2023.

关键词： Solid-state batteries Garnet electrolytes Air stability Interface engineering Lithium foil contamination

Revealing the Role of Defect in 3D Graphene-Based Photocatalytic Composite for Efficient Elimination of Antibiotic and Heavy Metal Combined Pollution

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Energy & Environmental Materials 2024年第3期7卷 164-174页

作者： Xin wang Jingzhe Zhang Hui wang Mengjun Liang Qiang wang Fuming Chen Research Institute of Frontier Science Southwest Jiaotong UniversityChengdu 610031China Guangdong Provincial Key Laboratory of Quantum Engineering and Quantum Materials School of Electronics and Information EngineeringSouth China Normal UniversityFoshan 528225China School of Aeronautics Northwestern Polytechnical UniversityXi'an 710072China Hubei Key Laboratory for High-Efficiency Utilization of Solar Energy and Operation Control of Energy Storage System Hubei University of TechnologyWuhan 430068China MOE Key Laboratory of Thermo-Fluid Science and Engineering School of Energy and Power EngineeringXi'an Jiaotong UniversityXi'an 710049China

Defect engineering can give birth to novel properties for adsorption and photocatalysis in the control of antibiotics and heavy metal combined pollution with photocatalytic ***,the role of defects and the process mechanism are complicated and ***,TiO_(2)/CN/3DC was fabricated and defects were introduced into the tripartite structure with separate O_(2)plasma treatment for the single *** find that defect engineering can improve the photocatalytic activity,attributing to the increase of the contribution from h^(+)and *** contrast to TiO_(2)/CN/3DC with a photocatalytic tetracycline removal rate of 75.2%,the removal rate of TC with D-TiO_(2)/CN/3DC has increased to 88.5%.Moreover,the reactive sites of tetracycline can be increased by adsorbing on the defective *** defect construction on TiO_(2)shows the advantages in tetracycline degradation and Cu^(2+)adsorption,but also suffers significant inhibition for the tetracycline degradation in a tetracycline/Cu^(2+)combined *** contrast,the defect construction on graphene can achieve the cooperative removal of tetracycline and Cu^(2+).These findings can provide new insights into water treatment strategies with defect engineering.

关键词： 3D graphene Cu defect photocatalytic composite tetracycline

Performance and mechanism of La-Fe metal-organic framework as a highly efficient adsorbent for fluoride removal from mine water

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Journal of Environmental Sciences 2024年第5期139卷 245-257页

作者： Chaomin Jia Jianbing wang Huijiao wang Sichao Zhu Xiaohui Zhang Yuxiang wang School of Chemical&Environmental Engineering China University of Mining&Technology-BeijingBeijing 100083China Beijing Polytechnic Beijing 100176China Chinese Society for Urban Studies Beijing 100835China

Water fluoride pollution has caused non-negligible harm to the environment and humans,and thus it is crucial to find a suitable treatment *** this study,La-Fe@PTA adsorbent was synthesized for the defluoridation of mine *** results showed that the optimum conditions for defluoridation by La-Fe@PTA were p H close to 7.0,the initial F-concentration of 10 mg/L,the dosage of 0.5 g/L and the adsorption time of 240 *** with SO_4^(2-),Cl^(-),NO_(3)^(-),Ca^(2+)and Mg^(2+),CO_(3)^(2-)and HCO_(3)^(-)presented severer inhibition on fluoride uptake by La-Fe@*** adsorption process fits well with the pseudo-second-order kinetic model and Freundlich model,and the maximum adsorption capacity of Langmuir model was 95 mg/***-bed adsorption results indicated that fluoride in practical fluorinated mine water could be effectively removed from 3.6 mg/L to less than 1.5 mg/L within130 bed volume(BV)by using 1.5 g La-Fe@***,the adsorbent still had good adsorption capacity after regeneration,which confirms the great application potential of La-Fe@PTA as a fluoride ion *** mechanism analysis showed that La-Fe@PTA adsorption of fluorine ions is a physicochemical reaction driven by electrostatic attraction and ion exchange.

关键词： Adsorption La-Fe@PTA Fluoride ion Mine water Mechanism