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Tuning electrochemical water activation over NiIr single-atom alloy aerogels for stable electrochemiluminescence

science Bulletin 2024年第15期69卷 2387-2394页

作者： Ling Ling Mengzhen Xi Hengjia Wang Runshi Xiao Lirong Zheng Liuyong Hu Wenling Gu Chengzhou Zhu State Key Laboratory of Green Pesticide International Joint Research Center for Intelligent Biosensing Technology and HealthCollege of ChemistryCentral China Normal UniversityWuhan 430079China Hubei Key Laboratory of Plasma Chemistry and advanced Materials Hubei Engineering Technology Research Center of Optoelectronic and New Energy MaterialsWuhan Institute of TechnologyWuhan 430205China Institute of High energy Physics Chinese Academy of SciencesBeijing 100049China

The anodic oxygen evolution reaction is a well-acknowledged side reaction in traditional aqueous electrochemiluminescence(ECL) systems due to the generation and surface aggregation of oxygen at the electrode, which detrimentally impacts the stability and efficiency of ECL emission. However, the effect of reactive oxygen species generated during water oxidation on ECL luminophores has been largely overlooked. Taking the typical luminol emitter as an example, herein, we employed NiIr single-atom alloy aerogels possessing efficient water oxidation activity as a prototype co-reaction accelerator to elucidate the relationship between ECL behavior and water oxidation reaction kinetics for the first time. By regulating the concentration of hydroxide ions in the electrolyte, the electrochemical oxidation processes of both luminol and water are finely tuned. When the concentration of hydroxide ions in electrolyte is low,the kinetics of water oxidation is attenuated, which limits the generation of oxygen, effectively mitigates the influence of oxygen accumulation on the ECL strength, and offers a novel perspective for harnessing side reactions in ECL systems. Finally, a sensitive and stable sensor for antioxidant detection was constructed and applied to the practical sample detection.

关键词： Electrochemiluminescence Luminol Water activation Single-atom doping Sensing

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Solar manipulations of perpendicular magnetic anisotropy for flexible spintronics

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Frontiers of physics 2024年第4期19卷 73-79页

作者： Zhexi He Yifan Zhao Yujing Du Meng Zhao Yuxuan Jiang Ming Liu Ziyao Zhou State Key Laboratory for Manufacturing Systems Engineering Electronic Materials Research LaboratoryKey Laboratory of the Ministry of Education&International Center for Dielectric ResearchSchool of Electronic Science and EngineeringThe International Joint Laboratory for Micro/Nano Manufacturing and Measurement TechnologyXi’an Jiaotong UniversityXi’an 710049China School of Materials science&Engineering Changzhou UniversityChangzhou 213164China

Flexible electronics/spintronics attracts researchers’attention for their application potential abroad in wearable devices,healthcare,and other *** devices’performance(speed,energy consumption)is highly dependent on manipulating information bits(spin-orientation in flexible spintronics).In this work,we established an organic photovoltaic(OPV)/ZnO/Pt/Co/Pt heterostructure on flexible PET substrates with perpendicular magnetic anisotropy(PMA).Under sunlight illumination,the photoelectrons generated from the OPV layer transfer into the PMA heterostructure,then they reduce the PMA strength by enhancing the interfacial Rashba field *** coercive field(Hc)reduces from 800 Oe to 500 Oe at its maximum,and the magnetization can be switched up and down *** stability of sunlight control of magnetization reversal under various bending conditions is also tested for flexible spintronic ***,the voltage output of sunlight-driven PMA is achieved in our prototype device,exhibiting an excellent angular dependence and opening a door towards solar-driven flexible spintronics with much lower energy consumption.

关键词： interfacial magnetoelectric coupling perpendicular magnetic anisotropy deterministic magnetization reversal photovoltaic control of magnetism

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Pulse-doubling perovskite nanowire lasers enabled by phonon-assisted multistep energy funneling

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Light(science & Applications) 2024年第8期13卷 1645-1654页

作者： Chunhu Zhao Jia Guo Jiahua Tao Junhao Chu Shaoqiang Chen Guichuan Xing Hunan Provincial Key Laboratory of Carbon Neutrality and Intelligent energy School of Resource&EnvironmentHunan University of Technology and Business410205 ChangshaChina Engineering research center for Nanophotonics and advanced Instrument Ministry of EducationSchool of Physics and Electronic ScienceEast China Normal University200241 ShanghaiChina Joint Key Laboratory of the Ministry of education Institute of Applied Physics and Materials EngineeringUniversity of Macao999078 MacaoChina

Laser pulse multiplication from an optical gain medium has shown great potential in miniaturizing integrated optoelectronic *** multiple quantum wells(MQWs)structures have recently been recognized as an effective gain media capable of doubling laser pulses that do not rely on external optical *** the light amplifications enabled with pulse doubling are reported based on the perovskite MQWs thin films,the micronanolasers possessed a specific cavity for laser pulse multiplication and their corresponding intrinsic laser dynamics are still ***,a single-mode double-pulsed nanolaser from self-assembled perovskite MQWs nanowires is realized,exhibiting a pulse duration of 28 ps and pulse interval of 22 ps based on single femtosecond laser pulse *** is established that the continuous energy building up within a certain timescale is essential for the multiple population inversion in the gain medium,which arises from the slowing carrier localization process owning to the stronger exciton–phonon coupling in the smaller-n ***,the double-pulsed lasing is achieved from one fast energy funnel process from the adjacent small-n QWs to gain active region and another slow process from the spatially separated *** report may shed new light on the intrinsic energy relaxation mechanism and boost the further development of perovskite multiple-pulse lasers.

关键词： doubling energy phonon

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Volumetric and viscometric properties of aqueous 1,2-dimethylethylenediamine solution for carbon capture application

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Petroleum 2024年第2期10卷 326-337页

作者： Hossein Haghani Teerawat Sema Pipat Na Ranong Thanthip Kiattinirachara Benjapon Chalermsinsuwan Hongxia Gao Zhiwu Liang Paitoon Tontiwachwuthikul Department of Chemical Technology Faculty of Science Chulalongkorn University center of Excellence on Petrochemical and Materials Technology Chulalongkorn University Department of Chemical Engineering Faculty of Engineering Mahidol University Joint international center for CO Clean energy Technologies research Institute (CETRi) Faculty of Engineering and Applied Science University of Regina

The present work investigates the volumetric and viscometric properties of an aqueous solution of 1,2-dimethylethylenediamine(DEEDA) over an entire concentration range and an absorber operating temperature range of 313.15K-333.15K at atmospheric pressure. The investigated volumetric properties included the density, excess molar volume, partial molar volume, and the investigated viscometric properties included the viscosity, viscosity deviation, free energy for activation of viscous flow, excess free energy for activation of viscous flow, and excess entropy for activation of viscous flow. The results indicated that there are strong intermolecular interactions and suitable molecular packing in the binary DEEDA-water mixture. Hence, the mixture was found to deviate from a real mixture according to the calculated excess properties. The DEEDA solvent's preliminary volumetric and viscometric properties revealed convincing potential as a novel amine for carbon capture. Additionally, the Redlich-Kister-based correlations showed favorable correlative performance for excess molar volume, viscosity deviation, and excess entropy for activation of viscous flow.

关键词： Density Viscosity Excess property Amine Carbon capture

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Coordination-environment regulation of atomic Co-Mn dual-sites for efficient oxygen reduction reaction

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Nano research 2024年第8期17卷 6841-6848页

作者： Caiting Sun Yarong Liu Zunhang Lv Rui Liu Changli Wang Liuhua Li Jinming Wang Yu Zhang Wenxiu Yang Bo Wang Key Laboratory of Cluster science(Ministry of education) Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion MaterialsAdvanced Technology Research Institute(Jinan)Advanced Research Institute of Multidisciplinary ScienceSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China Beijing Institute of Technology Library Beijing Institute of TechnologyBeijing 100081China

Precisely designing atomic metal-nitrogen-carbon(M-N-C)catalysts with asymmetric diatomic configurations and studying their structure–activity relationships for oxygen reduction reaction(ORR)are important for zinc-air batteries(ZABs).Herein,a dualatomic-site catalyst(DASC)with CoN_(3)S-MnN_(2)S_(2) configuration was prepared for the cathodes of *** with Co-N-C(Mn-free)and CoMn-N-C(S-free doping),CoMn-N/S-C exhibits excellent half-wave potential(0.883 V)and turnover frequency(1.54 e·s^(−1)·site^(−1)),surpassing most of the reported state-of-the-art Pt-free ORR *** CoMn-N/S-C-based ZABs achieve extremely high specific capacity(959 mAh·g^(−1))and good stability(350 h@5 mA·cm^(−2)).Density functional theory(DFT)calculation shows that the introduction of Mn and S can break the electron configuration symmetry of the original Co 3d orbital,lower the dband center of the Co site,and optimize the desorption behavior of*OH intermediate,thereby increasing the ORR activity.

关键词： metal organic frameworks oxygen reduction reaction dual-atom catalyst coordination-environment regulation zinc-air batteries

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Universal insertion of molecules in ionic compounds under pressure

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National science Review 2024年第1期11卷 120-128页

作者： Feng Peng Yanming Ma Chris J.Pickard Hanyu Liu Maosheng Miao College of Physics and Electronic Information Luoyang Normal University Department of Chemistry and Biochemistry California State University Northridge State Key Laboratory of Superhard Materials & Key Laboratory of Material Simulation Methods and Software of Ministry of education College of Physics Jilin University international center of Future science Jilin University Department of Materials science & Metallurgy University of Cambridge advanced Institute for Materials research Tohoku University Department of Earth science University of California Santa Barbara

Using first-principles calculations and crystal structure search methods, we found that many covalently bonded molecules such as H2, N2, CO2, NH3, H2O and CH4may react with NaC l, a prototype ionic solid,and form stable compounds under pressure while retaining their molecular structure. These molecules,despite whether they are homonuclear or heteronuclear, polar or non-polar, small or large, do not show strong chemical interactions with surrounding Na and Cl ions. In contrast, the most stable molecule among all examples, N2, is found to transform into cyclo-N5-anions while reacting with NaC l under high pressures. It provides a new route to synthesize pentazolates, which are promising green energy materials with high energy density. Our work demonstrates a unique and universal hybridization propensity of covalently bonded molecules and solid compounds under pressure. This surprising miscibility suggests possible mixing regions between the molecular and rock layers in the interiors of large planets.

关键词： molecule-solid hybrid materials high-pressure crystal structure prediction density functional theory planet interior

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Confinement of ionomer for electrocatalytic CO2 reduction reaction via efficient mass transfer pathways

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National science Review 2024年第2期11卷 168-176页

作者： Xiaowei Du Peng Zhang Gong Zhang Hui Gao Lili Zhang Mengmeng Zhang Tuo Wang Jinlong Gong School of Chemical Engineering and Technology Key Laboratory for Green Chemical Technology of the Ministry of Education Tianjin University Collaborative Innovation center of Chemical science and Engineering(Tianjin) National Industry-education Platform of energy Storage Tianjin University Joint School of the National University of Singapore and Tianjin University International Campus of Tianjin University Haihe Laboratory of Sustainable Chemical Transformations

Gas diffusion electrodes（GDEs） mediate the transport of reactants, products and electrons for the electrocatalytic CO2reduction reaction（CO2RR） in membrane electrode assemblies. The random distribution of ionomer, added by the traditional physical mixing method, in the catalyst layer of GDEs affects the transport of ions and CO2. Such a phenomenon results in elevated cell voltage and decaying selectivity at high current densities. This paper describes a pre-confinement method to construct GDEs with homogeneously distributed ionomer, which enhances mass transfer locally at the active centers. The optimized GDE exhibited comparatively low cell voltages and high CO Faradaic efficiencies（FE > 90%） at a wide range of current densities. It can also operate stably for over 220 h with the cell voltage staying almost unchanged. This good performance can be preserved even with diluted CO2feeds, which is essential for pursuing a high single-pass conversion rate. This study provides a new approach to building efficient mass transfer pathways for ions and reactants in GDEs to promote the electrocatalytic CO2RR for practical applications.

关键词： CO2 electroreduction gas diffusion electrode mass transfer ionomer Ag catalyst

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A perspective on the key factors of safety for rechargeable magnesium batteries

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Journal of energy Chemistry 2024年第7期94卷 656-676页

作者： Shuangshuang Tan Jie Xu Rongrui Deng Qiannan Zhao Chaohe Xu Guangsheng Huang Jingfeng Wang Fusheng Pan National Engineering research center for Magnesium Alloys Chongqing UniversityChongqing 400044China National Innovation center for Industry-education Integration of energy Storage Technology College of Materials Science and EngineeringChongqing UniversityChongqing 400044China Chongqing Institute of New energy Storage Materials and Equipment Chongqing 401135China

Rechargeable Mg batteries(RMBs)have become one of the best subsitutes for lithium-ion batteries due to the high volumetric capacity,abundant resources,and uniform plating behavior of Mg metal ***,the safety hazard induced by the formation of high-modulue Mg dendrites under a high current density(10 mA cm^(-1))was still revealed in recent *** has forced researchers to re-examine the safety of *** this review,the intrinsic safety factors of key components in RMBs,such as uneven plating,pitting and flammability of Mg anode,heat release and crystalline water decomposition of cathode,strong corrosion,low oxidition stability and flammability of electrolytes,and soforth,are systematacially *** origins,formation mechanisms,and possible safety hazards are deeply *** develop high-performance Mg anode,current strategies including designing artificial SEI,three-dimensional substrates,and Mg alloys are *** practical electrolytes,the configurations of boron-centered anions and simple Mg salts and the functionalized solvent with high boiling point and low flammability are suggested to comprehensively *** addition,the future study should more focus on the investigation on the thermal runaway and decomposition of cathode materials and *** review aims to provide fundamental insights into the relationship between electrochemistry and safety,further promoting the sustainable development of RMBs.

关键词： Rechargeable Mg batteries Battery safety Mg dendrites Electrolyte decomposition Intrinsic safety issues

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Seasonal prediction of extreme high-temperature days over the Yangtze River basin

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science China Earth sciences 2024年第7期67卷 2137-2147页

作者： Shifeng PAN Zhicong YIN Mingkeng DUAN Tingting HAN Yi FAN Yangyang HUANG Huijun WANG Key Laboratory of Meteorological Disaster Ministry of Education/Joint International Research Laboratory of Climate and Environment Change/Collaborative Innovation Center on Forecast and Evaluation of Meteorological DisastersNanjing University of Information Science and TechnologyNanjing 210044China Southern Marine science and Engineering Guangdong Laboratory(Zhuhai) Zhuhai 519080China

Extreme high temperatures occur frequently over the densely populated Yangtze River basin(YRB)in China during summer,significantly impacting the local economic development and ecological ***,accurate prediction of extreme high-temperature days in this region remains a ***,the Climate Forecast System Version 2(CFSv2)exhibits poor performance in this ***,based on the interannual increment approach,we develop a hybrid seasonal prediction model over the YRB(HM_(YRB))to improve the prediction of extreme high-temperature days in *** HM_(YRB)relies on the following four predictors:the observed preceding April-May snowmelt in north western Europe;the snow depth in March over the central Siberian Plateau;the CFSv2-forecasted concurrent summer sea surface temperatures around the Maritime Continent;and the 200-hPa geopotential height over the Tibetan *** HM_(YRB)indicates good capabilities in predicting the interannual variability and trend of extreme high-temperature days,with a markable correlation coefficient of 0.58 and a percentage of the same sign(PSS)of 76% during 1983-2015 in the one-year-out ***,the HM_(YRB) maintains high PSS skill(86%)and robustness in the independent prediction period(2016-2022).Furthermore,the HM_(YRB) shows a good performance for years with high occurrence of extreme high-temperature days,with a hit ratio of 40%.These predictors used in HM_(YRB)are beneficial in terms of the prediction skill for the average daily maximum temperature in summer over the YRB,albeit with biases existing in the *** study provides promising insights into the prediction of 2022-like hot extremes over the YRB in China.

关键词： Hot extremes Yangtze River basin CFSv2 Seasonal prediction One-year-out cross-validation

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Optimization of Product Distribution for MIP Units Using Data Mining

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China Petroleum Processing & Petrochemical Technology 2024年第2期26卷 146-157页

作者： Wang Qing Zhang Xiaoguo Mei Junwei Gao Zhibo Yang Kuizhi Yang Dawei Ouyang Fusheng international Joint research center of Green energy Chemical Engineering East China University of Science and TechnologyShanghai 200237China SINOPEC Changling Petrochemical Co. LtdYueyang 414012China

Based on data from a petrochemical company’s MIP unit over the past three years,19 input variables and 2 output variables were selected for modeling using the maximum information coefficient and Pearson correlation coefficient among 155 variables,which included properties of feedstock oil and spent catalyst,operational variables,and material *** distillation range variables were reduced using factor analysis,and the feedstock oils were clustered into three types using the K-means++*** feedstock oil type was then used as an input variable for *** XGBoost model and a back propagation(BP)neural network model with a structure of 20-15-15-2 were developed to predict the combined yield of gasoline and propylene,as well as the coke *** the test set,the BP neural network model demonstrated better fitting and generalization abilities with a mean absolute percentage error and determination coefficient of 1.48%and 0.738,respectively,compared to the XGBoost *** was therefore chosen for further optimization *** genetic algorithm was utilized to optimize operational variables in order to increase the combined yield of gasoline and propylene while controlling the growth of coke *** commercial test results in the MIP unit showed an average increase of 1.39 percentage points for the combined yield of gasoline and propylene and an average decrease of 0.11 percentage points for coke *** results indicate that the model effectively improves the combined yield of gasoline and propylene while controlling the increase in coke yield.

关键词： MIP process K-Means++ BP neural network model XGBoost algorithm genetic algorithm

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