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Recent advances and key perspectives of in-situ studies for oxygen evolution reaction in water electrolysis

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Green Energy & Environment 2024年第10期9卷 1497-1517页

作者： Yi wang Zichen Xu Xianhong wu Zhong-Shuai wu State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences Shijingshan District Dalian National Laboratory for Clean Energy Chinese Academy of Sciences

Electricity-driven water splitting to produce hydrogen is one of the most efficient ways to alleviate energy crisis and environmental pollution problems, in which the anodic oxygen evolution reaction(OER) is the key half-reaction of performance-limiting in water splitting. Given the complicated reaction process and surface reconstruction of the involved catalysts under actual working conditions, unraveling the real active sites, probing multiple reaction intermediates and clarifying catalytic pathways through in-situ characterization techniques and theoretical calculations are essential. In this review, we summarize the recent advancements in understanding the catalytic process, unlocking the water oxidation active phase and elucidating catalytic mechanism of water oxidation by various in-situ characterization techniques. Firstly, we introduce conventionally proposed traditional catalytic mechanisms and novel evolutionary mechanisms of OER, and highlight the significance of optimal catalytic pathways and intrinsic stability. Next, we provide a comprehensive overview of the fundamental working principles,different detection modes, applicable scenarios, and limitations associated with the in-situ characterization techniques. Further, we exemplified the in-situ studies and discussed phase transition detection, visualization of speciation evolution, electronic structure tracking, observation of reaction active intermediates, and monitoring of catalytic products, as well as establishing catalytic structure–activity relationships and catalytic mechanism. Finally, the key challenges and future perspectives for demystifying the water oxidation process are briefly proposed.

关键词： In-situ studies Water splitting Oxygen evolution reaction Catalytic mechanism

The reformation of catalyst:From a trial-and-error synthesis to rational design

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Nano Research 2024年第4期17卷 3261-3301页

作者： Ligang wang Jiabin wu Shunwu wang Huan Liu Yao wang Dingsheng wang Department of Chemistry Tsinghua UniversityBeijing 100084China

The appropriate catalysts can accelerate the reaction rate and effectively boost the efficient conversion of various molecules,which is of great importance in the study of chemistry,chemical industry,energy,materials and environmental ***,efficient,environmentally friendly,and easy to operate synthesis methods have been used to prepare various types of *** previous studies have reported the synthesis and characterization of the aforementioned catalysts,more still remain in trial and error methods,without in-depth consideration and improvement of traditional synthesis ***,we comprehensively summarize and compare the preparation methods of the trial-and-error synthesis strategy,structure–activity relationships and density functional theory(DFT)guided catalysts rational design for nanomaterials and atomically dispersed *** also discuss in detail the utilization of the nanomaterials and single atom catalysts for converting small molecules(H_(2)O,O_(2),CO_(2),N_(2),etc.)into value-added products driven by electrocatalysis,photocatalysis,and ***,the challenges and outlooks of mass preparation and production of efficient and green catalysts through conventional trial and error synthesis and DFT theory are featured in accordance with its current development.

关键词： trial-and-error synthesis structure–activity relationships density functional theory(DFT)guidance nanomaterials atomically dispersed catalysts

Extending the detection limit:innovations in infrared quantum dot photodetectors reaching up to 18μm

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Light(Science & Applications) 2024年第8期13卷 1445-1447页

作者： Chong wu wang Qi Jie wang Centre for OptoElectronics and Biophotonics School of Electrical and Electronic EngineeringNanyang Technological UniversitySingapore 639798Singapore Centre for Disruptive Photonic Technologies School of Physical and Mathematical SciencesNanyang Technological UniversitySingaporeSingapore

A regrowth method was used to synthesize large-sized colloidal quantum dots(CQDs).With the assistance of doping engineering,the synthesized CQD detectors demonstrate exceptional long-wavelength infrared detection performance,reaching up to 18μm,significantly extending the spectral response limit for CQD-based infrared *** detectors also achieve a reasonably high detectivity of 6.6×10^(8)Jones.

关键词： limit quantum sized

Some Convergence Properties for Weighted Sums of Martingale Difference Random Vectors

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Acta Mathematica Sinica,English Series 2024年第4期40卷 1127-1142页

作者： Yi wu Xue Jun wang School of Big Data and Artificial Intelligence Chizhou UniversityChizhou 247000P.R.China School of Big Data and Statistics Anhui UniversityHefei 230601P.R.China

Let{X_(ni),F_(ni);1≤i≤n,n≥1}be an array of R^(d)martingale difference random vectors and{A_(ni),1≤i≤n,n≥1}be an array of m×d matrices of real *** this paper,the Marcinkiewicz-Zygmund type weak law of large numb... 详细信息

关键词： Martingale difference random vectors weighted sums Marcinkiewicz–Zygmund type weak law of large numbers complete convergence strong law of large numbers multivariate simple linear regression model

Reconcile the contradictory wettability requirements for the reduction and oxidation half-reactions in overall CO_(2) photoreduction via alternately hydrophobic surfaces

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Journal of Energy Chemistry 2024年第6期93卷 202-212,I0006页

作者： Hailing Huo Ting Hu Chengxi Huang Fang wu Tongyu wang Xuan Liu Liang Zhang Qiang Ju Zhiqing Zhong Hongbin xing Erjun Kan Ang Li MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing Nanjing University of Science and TechnologyNanjing 210094JiangsuChina College of Information Science and Technology Nanjing Forestry UniversityNanjing 210037JiangsuChina

The overall photocatalytic CO_(2) reduction reaction(OPCRR)that can directly convert CO_(2) and H_(2)O into fuels represents a promising renewable energy conversion *** a typical redox reaction,the OPCRR involves two half-reactions:the CO_(2) reduction half-reaction(CRHR)and the water oxidation half-reaction(WOHR).Generally,both half-reactions can be promoted by adjusting the wettability of ***,there is a contradiction in wettability requirements for the two ***,CRHR prefers a hydrophobic surface that can accumulate more CO_(2) molecules on the active sites,ensuring the appropriate ratio of gas-phase(CO_(2))to liquid-phase(H_(2)O)***,the WOHR prefers a hydrophilic surface that can promote the departure of the gaseous product(O_(2))from the catalyst surface,preventing isolation between active sites and the reactant(H_(2)O).Here,we successfully reconciled the contradictory wettability requirements for the CRHR and WOHR by creating an alternately hydrophobic *** was achieved through a selectively hydrophobic modification method and a charge-transfer-control ***,the collaboratively promoted CRHR and WOHR led to a significantly enhanced OPCRR with a solar-to-fuel conversion efficiency of 0.186%.Notably,in ethanol production,the catalyst exhibited a 10.64-fold increase in generation rate(271.44μmol g^(-1)h~(-1))and a 4-fold increase in selectivity(55.77%)compared to the benchmark *** innovative approach holds great potential for application in universal overall reactions involving gas participation.

关键词： Hydrophobic Hydrophilic Gas transport Overall CO_(2)photoreduction Z-scheme

Novel high-voltage cathode for aqueous zinc ion batteries:Porous K_(0.5)VOPO_(4)·1.5H_(2)O with reversible solid-solution intercalation and conversion storage mechanism

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Journal of Energy Chemistry 2024年第6期93卷 71-78,I0003页

作者： Liyu wang Mingliang Zhao Xiaoyu Zhang Menghua wu Yu Zong Yu Chen Xinliang Huang Mingjie xing Xin Ning Wen Wen Daming Zhu Xiaochuan Ren Industrial Research Institute of Nonwovens&Technical Textiles College of Textiles&ClothingShandong Engineering Research Center for Specialty Nonwoven MaterialsQingdao UniversityQingdao 266071ShandongChina Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China

Cathode materials that possess high output voltage,as well as those that can be mass-produced using facile techniques,are crucial for the advancement of aqueous zinc-ion battery(ZIBs)applications,Herein,we present for the first time a new porous K_(0.5)VOPO_(4)·1.5H_(2)O polyanionic cathode(P-KIVP)with high output voltage(above 1.2 V)that can be manufactured at room temperature using straightforward coprecipitation and etching *** P-KVP cathode experiences anisotropic crystal plane expansion via a sequential solid-solution intercalation and phase co nversion pathway throughout the Zn^(2+)storage process,as confirmed by in-situ synchrotron X-ray diffraction and ex-situ X-ray photoelectron *** to other layered vanadium-based polyanionic materials,the P-KVP cathode experiences a progressive decline in voltage during the cycle,which is demonstrated to be caused by the irreversible conversion into amorphous VO_(x).By introducing a new electrolyte containing Zn(OTF)_(2) to a mixed triethyl phosphate and water solution,it is possible to impede this irreversible conversion and obtain a high output voltage and longer cycle life by forming a P-rich cathode electrolyte interface *** a proof-of-concept,the flexible fiber-shaped ZIBs based on modified electrolyte woven into a fabric watch band can power an electronic watch,highlighting the application potential of P-KVP cathode.

关键词： Aqueous zinc ion battery Cathode Porous material High voltage platform In-situ synchrotron X-ray diffraction

Thermal transports in the MXenes family:Opportunities and challenges

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Nano Research 2024年第8期17卷 7700-7716页

作者： Yurui Liu Yue wu Xinwei wang Department of Chemical and Biological Engineering Iowa State University618 Bissell AmesIA 50011USA Department of Mechanical Engineering 271 Applied Science Complex II1915 Scholl RoadIowa State UniversityAmesIA 50011USA

The carbides and nitrides of transition metals known as“MXenes”refer to a fast-growing family of two-dimensional materials discovered in *** to their unique nanolayer structure,superior electrical,mechanical,and thermal properties,MXenes have shown great potential in addressing the critical overheating issues that jeopardize the performance,stability,and lifetime of high-energy-density components in modern devices such as microprocessors,integrated circuits,and capacitors,*** outstanding intrinsic thermal conductivity of MXenes has been proved by experimental and theoretical *** MXenes-enabled high thermal conductivity composites incorporated with polymer matrix have also been reported and widely used as thermal management *** the booming heat dissipation demands,MXenes-enabled thermal management material is an extremely valuable and scalable option for modern electronics ***,the fundamental thermal transport mechanisms behind the MXenes family remain *** MXene thermal conductivity disparities between the theoretical prediction and experimental results are still *** better understand the thermal conduction in MXenes and provide more insights for engineering high-performance MXene thermal management materials,in this article,we summarize recent progress on thermal conductive *** essential factors that affect MXenes intrinsic thermal conductivities are tackled,selected MXenes-polymer composites are highlighted,and prospects and challenges are also discussed.

关键词： transition metal carbide(MXene) thermal transport two-dimensional materials thermally conductive composites

Saturation Estimation with Complex Electrical Conductivity for Hydrate-Bearing Clayey Sediments:An Experimental Study

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Journal of Ocean University of China 2024年第1期23卷 173-189页

作者： xing Lanchang ZHANG Shuli ZHANG Huanhuan wu Chenyutong wang Bin LAO Liyun WEI Wei HAN Weifeng WEI Zhoutuo GE Xinmin DENG Shaogui College of Control Science and Engineering China University of Petroleum(East China)Qingdao 266580China School of Water Energy and EnvironmentCranfield UniversityCranfield MK430ALUnited Kingdom Department of Alternative Energy PetroChina Research Institute of Petroleum Exploration&DevelopmentLangfang 065007China School of Geosciences China University of Petroleum(East China)Qingdao 266580China Laboratory for Marine Mineral Resources Qingdao National Laboratory for Marine Science and TechnologyQingdao 266071China

Clays have considerable influence on the electrical properties of hydrate-bearing *** is desirable to understand the electrical properties of hydrate-bearing clayey sediments and to build hydrate saturation(S_(h))models for reservoir evaluation and *** electrical properties of tetrahydrofuran-hydrate-bearing sediments with montmorillonite are characterized by complex conductivity at frequencies from 0.01 Hz to 1 *** effects of clay and Sh on the complex conductivity were analyzed.A decrease and increase in electrical conductance result from the clay-swelling-induced blockage and ion migration in the electrical double layer(EDL),*** quadrature conductivity increases with the clay content up to 10%because of the increased surface site density of counterions in *** the in-phase conductivity and quadrature conductivity decrease consistently with increasing Sh from 0.50 to *** sets of models for Sh evaluation were *** model based on the Simandoux equation outperforms Archie’s formula,with a root-mean-square error(E_(RMS))of 1.8%and 3.9%,respectively,highlighting the clay effects on the in-phase *** fre-quency effect correlations based on in-phase and quadrature conductivities exhibit inferior performance(E_(RMS)=11.6%and 13.2%,re-spectively)due to the challenge of choosing an appropriate pair of frequencies and intrinsic uncertainties from two *** second-order Cole-Cole formula can be used to fit the complex-conductivity *** pair of inverted Cole-Cole parameters,i.e.,characteristic time and chargeability,is employed to predict S_(h) with an E_(RMS) of 5.05%and 9.05%,respectively.

关键词： gas hydrate complex electrical conductivity hydrate-bearing clayey sediment hydrate saturation Simandoux equation frequency dispersion Cole-Cole formula

Effective Identity Authentication Based on Multiattribute Centers for Secure Government Data Sharing

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Tsinghua Science and Technology 2024年第3期29卷 736-752页

作者： Meiquan wang Junhua wu Tongdui Zhang Junhao wu Guangshun Li School of Computer Science Qufu Normal UniversityRizhao 276800China Science and Technology Innovation Service Institution of Rizhao Rizhao 276800China

As one of the essential steps to secure government data sharing,Identity Authentication(IA)plays a vital role in the processing of large ***,the centralized IA scheme based on a trusted third party presents problems of information leakage and single point of failure,and those related to key ***,herein,an effective IA model based on multiattribute centers is ***,a private key of each attribute of a data requester is generated by the attribute authorization *** obtaining the private key of attribute,the data requester generates a personal private ***,a dynamic key generation algorithm is proposed,which combines blockchain and smart contracts to periodically update the key of a data requester to prevent theft by external attackers,ensure the traceability of IA,and reduce the risk of privacy ***,the combination of blockchain and interplanetary file systems is used to store attribute field information of the data requester to further reduce the cost of blockchain information storage and improve the effectiveness of information *** results show that the proposed model ensures the privacy and security of identity information and outperforms similar authentication models in terms of computational and communication costs.

关键词： blockchain identity authentication distribution dynamic key generation