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Engineering tantalum nitride for efficient photoelectrochemical water splitting

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Science China Chemistry 2024年第7期67卷 2171-2180页

作者： beibei Zhang Zeyu Fan Yanbo Li Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054China

Photoelectrochemical(PEC)water splitting is a promising energy conversion strategy for directly converting solar energy into green hydrogen fuel.Constructing an efficient PEC device,finding an efficient photoanode material with a suitable band gap and favorable band-edge positions is essential.Tantalum nitride(Ta_(3)N_(5))meets these fundamental requirements,and its theoretical maximum solar-to-hydrogen(STH)conversion efficiency can reach 15.9%.Consequently,it has been widely applied as a photoanode material for the PEC oxygen evolution reaction(OER).However,severe bulk and interface charge recombination,along with sluggish water oxygen kinetics,seriously limits its STH conversion efficiency for PEC water splitting.Herein,this feature article briefly reviews recent advances by our research group in improving the STH conversion efficiency of the Ta_(3)N_(5)photoanode using various strategies,including defect engineering,construction of a gradient band structure,interface engineering,and surface modification of self-healing OER cocatalyst.Up to now,the obtained half-cell STH efficiency has exceeded 4%,providing a solid foundation for the development of tandem PEC devices for unbiased solar-driven overall water splitting toward practical application.

关键词： Photoelectrochemical water splitting tantalum nitride defect engineering interface engineering oxygen evolution cocatalyst

Global well-posedness for 2D inhomogeneous asymmetric fluids with large initial data

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Science China Mathematics 2024年第3期67卷 527-556页

作者： Chenyin Qian beibei He Ting Zhang School of Mathematical Sciences Zhejiang Normal UniversityJinhua 321004China School of Mathematical Sciences Zhejiang UniversityHangzhou 310058China

In this paper, by using time-weighted global estimates and the Lagrangian approach, we first investigate the global existence and uniqueness of the solution for the 2D inhomogeneous incompressible asymmetric fluids wi... 详细信息

关键词： inhomogeneous asymmetric fluids Littlewood-Paley theory Besov spaces global well-posedness

Effect of Direct Aging on Corrosion Behavior of AlSi10Mg Alloy Fabricated by Laser Powder Bed Fusion

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Acta Metallurgica Sinica(English Letters) 2024年第2期37卷 266-282页

作者： Zhen Zhang Zhanyong Zhao Xiaofeng Li beibei Wang Peikang Bai Shanxi Key Laboratory of Controlled Metal Solidification and Precision Manufacturing School of Materials Science and EngineeringNorth University of ChinaTaiyuan030051China Technical Center Taiyuan Iron and Steel(Group)Co.LtdTaiyuan030003China School of Materials Science and Engineering Taiyuan University of Science and TechnologyTaiyuan030024China

Effect of direct aging of 170℃on corrosion behavior of laser powder bed fused AlSi10Mg(LPBF-AlSi10Mg)was studied by microstructure analysis,electrochemical analysis and X-ray photoelectron spectrometer.The results show that direct aging of 170℃has little effect on melt pool and Si cellular structure,but promotes the precipitation of nano-Si particles and releases the residual stress.With increasing aging time from 0 to 4 h to 24 h,the corrosion property of the LPBF-AlSi10Mg is deteriorated,which is evidenced by increased corrosion current density and decreased pitting potential and polarization resistance.With increasing the aging time,the thickness of the oxide film formed on surface of the LPBF-AlSi10Mg increases.The Si content of the oxide film of the sample aging for 4 h is the lowest,9.42 at.%,and it is the highest,18.62 at.%,for the sample aging for 24 h.The electrochemical noise analysis reveals that the middle-frequency contribution of the Hilbert spectrum is responsible for the deteriorated corrosion performance,which corresponds to metastable pitting initiated by nano-Si particles.

关键词： Laser powder bed fusion AlSi10Mg Direct aging Corrosion

Deflagration characteristics of freely propagating flames in magnesium hydride dust clouds

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Defence Technology（防务技术） 2024年第1期31卷 471-483页

作者： Qiwei Zhang Yangfan Cheng beibei Zhang Danyi Li Zhaowu Shen School of Chemical Engineering Anhui University of Science and TechnologyHuainan 232001AnhuiPR China School of Civil Engineering and Architecture Anhui University of Science and TechnologyHuainan 232001AnhuiPR China Anhui Engineering Laboratory of Explosive Materials and Technology Anhui University of Science and TechnologyHuainan 232001AnhuiPR China School of Engineering Science University of Science and Technology of ChinaHefei 230027AnhuiPR China

The flame propagation processes of MgH_(2)dust clouds with four different particle sizes were recorded by a high-speed camera.The dynamic flame temperature distributions of MgH_(2)dust clouds were reconstructed by the two-color pyrometer technique,and the chemical composition of solid combustion residues were analyzed.The experimental results showed that the average flame propagation velocities of 23μm,40μm,60μm and 103μm MgH_(2)dust clouds in the stable propagation stage were 3.7 m/s,2.8 m/s,2.1 m/s and 0.9 m/s,respectively.The dust clouds with smaller particle sizes had faster flame propagation velocity and stronger oscillation intensity,and their flame temperature distributions were more even and the temperature gradients were smaller.The flame structures of MgH_(2)dust clouds were significantly affected by the particle sinking velocity,and the combustion processes were accompanied by micro-explosion of particles.The falling velocities of 23μm and 40μm MgH_(2)particles were 2.24 cm/s and 6.71 cm/s,respectively.While the falling velocities of 60μm and 103μm MgH_(2)particles were as high as 15.07 cm/s and 44.42 cm/s,respectively,leading to a more rapid downward development and irregular shape of the flame.Furthermore,the dehydrogenation reaction had a significant effect on the combustion performance of MgH_(2)dust.The combustion of H_(2)enhanced the ignition and combustion characteristics of MgH_(2)dust,resulting in a much higher explosion power than the pure Mg dust.The micro-structure characteristics and combustion residues composition analysis of MgH_(2)dust indicated that the combustion control mechanism of MgH_(2)dust flame was mainly the heterogeneous reaction,which was affected by the dehydrogenation reaction.

关键词： Magnesium hydride dust Flame combustion mechanism Particle size Dust explosion Two-color pyrometer

Active MoS_(2)-based electrode for green ammonia synthesis

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Chinese Journal of Chemical Engineering 2024年第1期65卷 268-275页

作者： Xin Liu Lei Yang Tao Wei Shanping Liu beibei Xiao School of Energy and Power Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China Institute Charles Gerhardt Montpellier UMR-5253Universite de MontpellierCNRSENSCMPlace E.Bataillon34095 Montpellier Cedex 05France

Nitrogen electro-reduction under mild conditions is one promising alternative approach of the energyconsuming Haber-Bosch process for the artificial ammonia synthesis.One critical aspect to unlocking this technology is to discover the catalysts with high selectivity and efficiency.In this work,the N_(2)-to-NH_(3)conversion on the functional MoS_(2)is fully investigated by density functional theory calculations since the layered MoS_(2)provides the ideal platform for the elaborating copies of the nitrogenase found in nature,wherein the functionalization is achieved via basal-adsorption,basal-substitution or edge-substitution of transition metal elements.Our results reveal that the edge-functionalization is a feasible strategy for the activity promotion;however,the basal-adsorption and basal-substitution separately suffer from the electrochemical instability and the NRR inefficiency.Specifically,MoS_(2)functionalized via edge W-substitution exhibits an exceptional activity.The energetically favored reaction pathway is through the distal pathway and a limiting potential is less than 0.20 V.Overall,this work escalates the rational design of the high-effective catalysts for nitrogen fixation and provides the explanation why the predicated catalyst have a good performance,paving the guidance for the experiments.

关键词： Nitrogen reduction reaction Density functional theory calculations Molybdenum disulfide Electrochemistry Catalyst Thermodynamics

Application of X-ray absorption spectroscopy in carbon-supported electrocatalysts

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Nano Research 2023年第11期16卷 12438-12452页

作者： beibei sheng Yongheng Chu Dengfeng Cao Yujian Xia Chongjing Liu Shuangming Chen Li Song National Synchrotron Radiation Laboratory CAS Center for Excellence in NanoscienceUniversity of Science and Technology of ChinaHefei 230026China

Breakthroughs in energy storage and conversion devices depend heavily on the exploration of low-cost and high-performance materials.Carbon-supported electrocatalysts with dimensional varieties have recently attracted significant attention due to their strong structural flexibility and easy accessibility.Nevertheless,understanding the connection between their electronic,structural properties,and catalytic performance must remain a top priority.Synchrotron radiation(SR)X-ray absorption spectroscopy(XAS)techniques,including hard XAS and soft XAS,are recognized as efficient and comprehensive platforms for probing the surface,interface,and bulk electronic structure of elements of interest in the materials community.In the past decade,the flourishing development of materials science and advanced characterization technologies have led to a deeper understanding at different temporal,longitudinal,and spatial scales.In this review,we briefly describe the concept of XAS techniques and summarize their recent progress in addressing scientific questions on carbon-supported electrocatalysts through the development of advanced instruments and experimental methods.We then discuss the remaining challenges and potential research directions in nextgeneration materials frontiers,and suggest challenges and perspectives for shedding light on the structure–activity relationship.

关键词： synchrotron radiation hard X-ray absorption spectroscopy(XAS) soft XAS carbon-supported electrocatalysts

NIR-Ⅱ responsive Janus nanoparticles amplify immunogenic cell death for enhanced cancer immunotherapy

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Science China(Technological Sciences) 2024年第1期67卷 321-329页

作者： CHEN beibei GUO KangLi WANG HaoRan XU Fu-Jian WANG JuLin ZHAO NaNa State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China Key Laboratory of Biomedical Materials of Natural Macromolecules(Beijing University of Chemical Technology) Beijing Laboratory of Biomedical MaterialsBeijing University of Chemical TechnologyBeijing 100029China College of Materials Sciences and Engineering Beijing University of Chemical TechnologyBeijing 100029China Beijing Key Laboratory of Electrochemical Process and Technology for Materials Beijing University of Chemical TechnologyBeijing 100029China

Immunotherapy brings new hope for tumor treatment by inducing immunogenic cell death(ICD)of tumor cells.However,insufficient immunogenicity and low immune response rate greatly limit antitumor immunity.Herein,by optimizing the composition and morphology,the rational design of Janus nanoparticles composed of Fe_(3)O_(4) nanospheres and SiO_(2)nanorods was realized for enhanced cancer immunotherapy through amplified ICD.After glucose oxidase(GOx)was loaded by the Janus nanoparticles,the resultant M-FS-GOx consumes glucose at tumor sites to generate gluconic acid and hydrogen peroxide(H_(2)O_(2))for starvation therapy while the H_(2)O_(2)supply promotes the production of highly toxic·OH to achieve effective chemodynamic therapy(CDT).Under a 1064 nm light irradiation,the photothermal effect of M-FS-GOx enhances the enzyme activity of GOx for improved starvation therapy.Furthermore,both tumor-associated antigens released during the process of ICD and the intrinsic immunoadjuvant property of M-FS-GOx stimulate dendritic cell maturation to activate antitumor immune responses.This work provides a promising strategy for the construction of Janus nanoparticles to achieve enhanced cancer immunotherapy through combination therapy-amplified ICD.

关键词： Janus nanoparticles immunogenic cell death cancer immunotherapy

A complementary binary code based phase unwrapping method

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Optoelectronics Letters 2024年第4期20卷 228-233页

作者： LI Wenjie SUN Huanghe LI Fuquan WANG beibei WANG Haijian GAO Xinyu School of Mechanical and Electrical EngineeringGuilin University of Electronic Technology Guilin 541004China

Phase unwrapping is used to establish the mapping relationship between camera and projector,which is one of the key technologies in fringe projection profilometry(FPP)based three-dimensional(3D)measurement.Although complementary Gray code assisted phase unwrapping technology can get a good result on the periodic boundary,it needs more coded images to obtain a high frequency fringe.Aiming at this problem,a complementary binary code assisted phase unwrapping method is proposed in this paper.According to the periodic consistency between the wrapping phase and binary codes,the coded patterns are generated.Then the connected domain strategy is performed to calculate the fringe orders using the positive and negative image binaryzation.To avoid the mistake near the periodic boundary,complementary binary code inspired by the complementary Gray code is proposed.The fringe order correction is also discussed for different situations in the first measured period.Only two binary images are needed in the proposed method,and the fringe frequency is not limited.Both the simulation and experiment have verified the feasibility of proposed method.

关键词： method. complementary phase

NbB_(2)Modified Al-Cu Alloys Fabricated by Freeze-Ablation Casting under High Cooling Rate Solidification

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Acta Metallurgica Sinica(English Letters) 2024年第5期37卷 921-938页

作者： Xiang Kong Yu Wang Hong Xu Haotian Fan Yuewu Zheng beibei Xie School of Materials Science and Engineering North University of ChinaTaiyuan 030051China

At present,improving the properties of aluminum alloys is generally achieved by increasing the cooling rate of the melt and adding micro-nano particles.Controlling the cooling rate of the melt to improve the refining effect of grain refiner is still a difficult problem in the aluminum alloy casting industry.An innovative and environmentally friendly casting process,known as freeze ablation,was introduced during the preparation of an Al–NbB_(2) intermediate alloy.This process significantly enhanced the cooling rate of the melt.The results indicated that the Al–NbB_(2) intermediate alloy produced under high cooling rates had a noticeable refining effect on Al–Cu alloys,with smaller NbB2 particles demonstrating superior refining performance.The average grain size of the refined Al–Cu alloy decreased from 154 to 69μm,the tensile strength increased by 12%,the fluidity increased by 18.4%,and the hot tearing index decreased from 144 to 12.The matching degree between NbB_(2) andα-Al was calculated using high-resolution transmission electron microscopy and the edge-to-edge model.It was found that the atomic interplanar spacing and the interatomic spacing mismatch between NbB_(2)’splane and Al were both less than 10%,which further proved that NbB2 could serve as an effective nucleation site forα-Al grains to achieve grain refinement.

关键词： Grain refinement Freeze ablation Particle size control Mechanical properties Process properties