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Efficient electroreduction of NO 3 - to NH 3 via the tandem catalysis of CeO x /B-Cu 2 O NWs

Applied Catalysis B: Environment and Energy 2025年 378卷

作者： Zhimin Yao Changzheng Lin Jiaxiang Gao Jiangtao Feng Mingtao Li Wei Yan Wenlong Zhang Hongjie Wang Hebei Key Laboratory of Close-to-Nature Restoration Technology of Wetlands School of Eco-Environment Hebei University Baoding 071002 China Department of Environmental Science & Engineering School of Energy and Power Engineering Xi’an Jiaotong University 28 Xianning West Road Xi’an 710049 China International Research Center for Renewable Energy (IRCRE) State Key Laboratory of Multiphase Flow in Power Engineering (MFPE) Xi’an Jiaotong University 28 Xianning West Road Xi’an 710049 China Engineering Research Center of Ecological Safety and Conservation in Beijing-Tianjin-Hebei (Xiong’an New Area) of MOE China

Electrocatalytic nitrate reduction (eNitRR) has emerged as a carbon-free method for sustainable ammonia synthesis and wastewater treatment. However, the complex reaction intermediates and sluggish hydrogenation kinetics remain the key barriers of eNitRR. Herein, this work presented tandem catalysis strategy and developed a B-doped Cu 2 O nanowires decorated with CeO x to address the two critical issues. Our work presents a high-performance CeO x /B-Cu 2 O NWs catalyst for eNitRR, achieving an ammonia yield of 2.137 mmol h −1 cm −2 and a Faraday efficiency of 98.8 %, which are superior to those of most previously reported catalysts. At a voltage of −0.5 V vs. RHE, cyclic tests with 8 cycles verified the exceptional stability of the catalyst. In-depth in-situ characterization and density functional theory (DFT) computations demonstrated that doping with boron (B) enhances the adsorption of *NO 3 due to the interactions between metallic and non-metallic components. Subsequently, the incorporation of CeO x modifies the electronic structure of Cu 2 O, thereby promoting hydrolysis and ensuring a sufficient supply of active hydrogen. Moreover, we report the successful development of an innovative Zn-NO 3 battery, demonstrating remarkable performance characteristics with an open-circuit voltage of 1.182 V and an exceptional peak power density reaching 21.91 mW cm −2 . Furthermore, by integrating eNitRR with an air stripping process, we successfully recovered high-purity NH 4 Cl products, providing a practical pathway for converting nitrate in wastewater into valuable ammonia-based products. This work provides comprehensive insights into the mechanism of tandem catalysis for eNitRR through the B doping and CeO x heterostructure.

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Electrochemical oxidation of rhodamine B by PbO_2/Sb-SnO_2/TiO_2 nanotube arrays electrode

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Chinese Journal of Catalysis 2019年第6期40卷 917-927页

作者： Jia Wu Kai Zhu Hao Xu Wei Yan Xi’an XD Switchgear Electric Co. Ltd.Xi’an 710049ShaanxiChina Department of Environmental Science and Engineering State Key Laboratory of Multiphase Flow in Power EngineeringXi’an Jiaotong UniversityXi’an 710049ShaanxiChina

A PbO2/Sb-SnO2/TiO2 nanotube array composite electrode was successfully synthesized and its electrochemical oxidation properties were ***-emission scanning electron microscopy(FE-SEM)and X-ray diffraction(XRD)results showed that the PbO2 coating was composed of anα-PbO2 inner layer and aβ-PbO2 outer *** life measurement indicated that the composite electrode had a lifetime of 815 *** B(RhB)was employed as a model pollutant to analyze the electrocatalytic activity of the *** effects of initial RhB concentration,current density,initial pH,temperature,and chloride ion concentration on the electrochemical oxidation were investigated in *** coupled plasma atomic emission spectroscopy(ICP-AES)results suggested that the concentration of leached Pb^2+in the electrolyte during the electrocatalytic oxidation process can be ***,the degradation mechanism during the electrocatalytic oxidation process was proposed based on the results of solid-phase micro-extraction-gas chromatography-mass spectrometry(SPME-GC-MS).The high electrocatalytic performance of the composite electrode makes it a promising anode for the treatment of organic pollutants in aqueous solution.

关键词： TiO2 nanotube array Electrochemical oxidation Rhodamine B Degradation mechanism

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Error Analysis of Liquid Holdup Measurement in Gas-Liquid Annular flow Through Circular Pipes Using High-Speed Camera Method

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Journal of Shanghai Jiaotong university(Science) 2018年第S1期23卷 34-40页

作者： LIU Li BAI Bofeng School of Nuclear Science and Engineering Shanghai Jiao Tong University State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University

Accurate measurement of gas-liquid phase fraction is essential for the proper modelling of the pressure drop, heat transfer coefficient, mass transfer rate and interfacial area in two-phase flows. In this paper, taking the issue of optical distortion into account, an analytical model was proposed to estimate and correct the liquid holdup in gas-liquid annular flow through a circular pipe using high-speed camera method. The error in the liquid holdup measurement generated from different refractive indices among transparent circular pipe, liquid film and air core was firstly theoretically analyzed based on the geometric optics. Experimental tests were then carried out to identify the difference as well as to validate the proposed model. Results indicated that the prediction of the liquid holdup has a good performance with the experimental data(i.e., mean relative error is 4.1%) and the measured liquid holdup is larger than the real one. It was found that the measured liquid holdup is larger than the real one. Generally, when the real liquid holdup gets smaller, the discrepancy between the measured liquid holdup by image and the real liquid holdup becomes more significant. Thus, after measuring the liquid holdup from the images, the value of the measured liquid holdup must be corrected by the present model in order to obtain the real liquid holdup.

关键词： gas-liquid annular flow liquid holdup optical refraction analytical correction

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Electrocatalytically Activating and Reducing N2Molecule by Tuning Activity of Local Hydrogen Radical

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Angewandte Chemie 2023年第20期135卷

作者： Yuanyuan Yang Cejun Hu Dr. Jieqiong Shan Chuanqi Cheng Prof. Lili Han Prof. Xinzhe Li Ruguang Wang Prof. Wei Xie Prof. Yao Zheng Prof. Tao Ling Key Laboratory for Advanced Ceramics and Machining Technology of Ministry of Education Tianjin Key Laboratory of Composite and Functional Materials School of Materials Science and Engineering Tianjin University Tianjin 300072 China Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Tianjin Key Lab of Molecular Recognition & Biosensing Renewable Energy Conversion and Storage Center College of Chemistry Nankai University Tianjin 300071 China School of Chemical Engineering The University of Adelaide Adelaide SA 5005 Australia State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 China State Key Laboratory of Multiphase Flow in Power Engineering School of Energy and Power Engineering Xi'an Jiaotong University Xi An Shi Xi'an 710049 China

Decarbonizing N 2 conversion is particularly challenging, but essential for sustainable development of industry and agriculture. Herein, we achieve electrocatalytic activation/reduction of N 2 on X/Fe−N−C (X=Pd, Ir and Pt) dual-atom catalysts under ambient condition. We provide solid experimental evidence that local hydrogen radical (H*) generated on the X site of the X/Fe−N−C catalysts can participate in the activation/reduction of N 2 adsorbed on the Fe site. More importantly, we reveal that the reactivity of X/Fe−N−C catalysts for N 2 activation/reduction can be well adjusted by the activity of H* generated on the X site, i.e., the interaction between the X−H bond. Specifically, X/Fe−N−C catalyst with the weakest X−H bonding exhibits the highest H* activity, which is beneficial to the subsequent cleavage of X−H bond for N 2 hydrogenation. With the most active H*, the Pd/Fe dual-atom site promotes the turnover frequency of N 2 reduction by up to 10 times compared with the pristine Fe site.

关键词： Carbon Materials Electrocatalysis Metal-Free Catalysts Nitrogen Reduction Reaction

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Combining Core-Shell Construction with Alloying Effect for High Efficiency Ethanol Electrooxidation: A Case of Core-Shell Au@Fepd Nanoparticles with Sub-Nano Alloy Shells

SSRN

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SSRN 2020年

作者： Liu, Danye Zeng, Qing Liu, Hui Hu, Chaoquan Chen, Dong Xu, Lin Yang, Jun State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China School of Chemistry and Materials Science Jiangsu Key Laboratory of New Power Batteries Nanjing Normal University Nanjing210023 China State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China

Combining the core-shell construction with an alloying effect is an effective way to optimize the electronic and lattice strain effects generated in core-shell configurations for achieving highly catalytic efficiency for a given electrochemical reaction. To demonstrate this concept, we herein report the use of core-shell Au@FePd nanoparticles with an Au core and a sub-nano FePd alloy shell to promote the electrocatalytic oxidation of ethanol. In these core-shell structures, the Au core modifies the electronic configuration of Pd atoms through differences in electronegativity, while the Fe component in thin shells reduces the lattice expansion of Pd induced by the Au core, both of which endows the Pd shell with an appropriate d-band center, favorable for the electrooxidation of ethanol molecules through C1 pathway. In particular, the as-prepared core-shell Au@FePd nanoparticles at an optimized Fe/Pd ratio of 0.5/1 (Au@FePd-0.5) exhibit a mass activity of 13.3 A mg-1 and a specific activity of 20.2 mA cm-2 for the ethanol electrooxidation in an alkaline medium, which significantly outperform those of a majority of the recent reported Pd-based electrocatalysts. This study highlights the concept of engineering the geometry and surface composition of a nanostructure for designing highly efficient electrocatalysts for a large variety of electrochemical applications. © 2020, The Authors. All rights reserved.

关键词： Shells (structures)

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Spin-to-orbital angular momentum conversion in non-Hermitian photonic graphene

arXiv

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arXiv 2025年

作者： Zhang, Zhaoyang Kokhanchik, Pavel Liu, Zhenzhi Shen, Yutong Liu, Fu Liu, Maochang Zhang, Yanpeng Xiao, Min Malpuech, Guillaume Solnyshkov, Dmitry Key Laboratory for Physical Electronics and Devices Ministry of Education Shaanxi Key Lab of Information Photonic Technique School of Electronic Science and Engineering Faculty of Electronics and Information Xi’an Jiaotong University Xi’an710049 China Institut Pascal PHOTON-N2 Université Clermont Auvergne CNRS Clermont INP Clermont-FerrandF-63000 France International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power Engineering Xi’an Jiaotong University Xi’an710049 China National Laboratory of Solid State Microstructures School of Physics Nanjing University Nanjing210093 China Paris75231 France

Optical beams with orbital angular momentum (OAM) have numerous potential applications, but the means used for their generation often lack crucial on-demand control. In this work, we present a mechanism of converting spin angular momentum (SAM) to OAM in a non-structured beam. The conversion occurs through spin-orbit coupling in a reconfigurable photonic honeycomb lattice with staggering implemented by electromagnetically-induced transparency in an atomic vapor cell. The spin-orbit coupling allows to outcouple the OAM signal from a particular band in a given valley determined by the chirality of light or the lattice staggering, providing a non-zero Berry curvature for generating OAM. The dependence of the output OAM on the chirality of the input beam is the first control knob. The staggering works as a second control knob, flipping the sign of OAM for the fixed chirality. The demonstrated conversion between SAM and OAM is important for optical communications. Our results can be extended to other implementations of paraxial photonic graphene. Copyright © 2025, The Authors. All rights reserved.

关键词： Angular momentum

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Enhanced efficiency in Concentrated Parabolic Solar Collector(CPSC) with a porous absorber tube filled with metal nanoparticle suspension

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Green Energy & Environment 2018年第2期3卷 129-137页

作者： Mohammad Hatami Jiafeng Geng Dengwei Jing Mechanical Engineering Department Esfarayen University of Technology (EUT) International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power EngineeringXi'an Jiaotong University

In this study, effects of different nanoparticles and porosity of absorber tube on the performance of a Concentrating Parabolic Solar Collector(CPSC) were investigated. A section of porous-filled absorber tube was modeled as a semi-circular cavity under the solar radiation which is filled by nanofluids and the governing equations were solved by FlexPDE numerical software. The effect of four physical parameters, nanoparticles type, nanoparticles volume fraction(φ), Darcy number(Da) and Rayleigh number(Ra), on the Nusselt number(Nu) was discussed. It turns out that Cu nanoparticle is the most suitable one for such solar collectors, compared to the commonly used Fe_3O_4, Al_2O_3, TiO_*** the increased addition of Cu nanoparticles all the parameters φ, Da and Ra shows a significant increase against the Nu, indicates the enhanced heat transfer in such cases. As a result, low concentration of Cu nanoparticle suspension combined with porous matrix was supposed to be beneficial for the performance enhancement of concentrating parabolic solar collector.

关键词： Concentrating parabolic solar collector Porous absorber tube Nanofluid Nusselt number Finite Element Method

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Theoretical Study on Photoacoustic Tweezers Based on Photo-Thermo-Acoustic-Mechanical Coupling Effects

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Zhongguo Jiguang/Chinese Journal of Lasers 2025年第9期52卷

作者： Lin, Zhanle Hu, Feifan Shan, Wanru Li, Dong Chen, Bin Zheng, Yuping Yao, Liang State Key Laboratory of Multiphase Flow in Power Engineering Xi’an Jiaotong University Shaanxi Xi’an710049 China Department of Ophthalmology The Second Affiliated Hospital Xi’an Jiaotong University Shaanxi Xi’an710004 China

Objective Photoacoustic tweezers (PATs) are a promising noninvasive technology for precise microparticle manipulation that leverage the photoacoustic effect to exert controlled forces on particles within a liquid medium. Conventional methods, such as optical and acoustic tweezers, present limitations such as potential damage to particles, inadequate spatial control, and restricted manipulation in three-dimensional (3D) environments. Hence, this study focuses on the theoretical development of a PAT model that integrates photo-thermo-acoustic-mechanical coupling effects. Using a ring-shaped laser beam, this study aims to investigate particle motion and force characteristics under various laser conditions. Additionally, this study seeks to establish a robust theoretical framework for PATs, thus filling the gaps in 3D particle manipulation and providing guidance for the optimization of experimental parameters. Methods A multiphysics coupling model for PATs was constructed to describe the interactions among photo-thermal, acoustic, and mechanical effects in a liquid medium. The model accounts for the transformation of laser energy density into heat and the subsequent thermal expansion, and the generation of acoustic waves that induces acoustic radiation forces and acoustic streaming. A ring-shaped laser beam was employed to create spatially confined acoustic fields that can trap and manipulate particles. Using the finite-element method (FEM) in Comsol software, the model was used to simulate high-frequency pulsed laser effects, including energy transfer, thermal expansion, acoustic wave propagation, and the resultant particle dynamics. The governing equations for the coupled fields were derived by incorporating the spatial and temporal distributions of the laser, the thermal and acoustic properties of the medium, and force interactions on the particles. The acoustic radiation forces were modeled based on Gor’kov potential theory, whereas the acoustic streaming fields wer

关键词： Acoustic emissions

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Tailoring Second Coordination Sphere for Tunable Solid–Liquid Interfacial Charge Transfer toward Enhanced Photoelectrochemical H2Production

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Angewandte Chemie 2024年第22期136卷

作者： Dr. Yangguang Hu Dr. Wu Zhou Dr. Wanbing Gong Prof. Chao Gao Prof. Shaohua Shen Prof. Tingting Kong Prof. Yujie Xiong Anhui Engineering Research Center of Carbon Neutrality The Key Laboratory of Functional Molecular Solids Ministry of Education College of Chemistry and Materials Science Anhui Normal University 241002 Wuhu Anhui China Hefei National Laboratory for Physical Sciences at the Microscale School of Chemistry and Materials Science University of Science and Technology of China 230026 Hefei Anhui China These authors equally contributed to this work International Research Centre for Renewable Energy State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University 710049 Xi'an Shaanxi China

The recombination of photogenerated charge carriers severely limits the performance of photoelectrochemical (PEC) H 2 production. Here, we demonstrate that this limitation can be overcome by optimizing the charge transfer dynamics at the solid–liquid interface via molecular catalyst design. Specifically, the surface of a p-Si photocathode is modulated using molecular catalysts with different metal atoms and organic ligands to improve H 2 production performance. Co(pda-SO 3 H) 2 is identified as an efficient and durable catalyst for H 2 production through the rational design of metal centers and first/second coordination spheres. The modulation with Co(pda-SO 3 H) 2 , which contains an electron-withdrawing −SO 3 H group in the second coordination sphere, elevates the flat-band potential of the polished p-Si photocathode and nanoporous p-Si photocathode by 81 mV and 124 mV, respectively, leading to the maximized energy band bending and the minimized interfacial carrier transport resistance. Consequently, both the two photocathodes achieve the Faradaic efficiency of more than 95 % for H 2 production, which is well maintained during 18 h and 21 h reaction, respectively. This work highlights that the band-edge engineering by molecular catalysts could be an important design consideration for semiconductor–catalyst hybrids toward PEC H 2 production.

关键词： PEC H2 production molecular catalyst coordination sphere surface modulation charge transfer

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Enhanced phase-transfer kinetics achieved by atomic iron catalysts on hard carbon toward low-temperature sodium-ion batteries

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Chemical engineering Journal 2025年

作者： Xinyi Qian Ziling Wu Jianan Gu Yanli Wang Xiaomin Cheng Jing Zhang Hongzhen Lin Jian Wang Liang Zhan Yongzheng Zhang State Key Laboratory of Green Chemical Engineering and Industrial Catalysis State Key Laboratory of Chemical Engineering Key Laboratory of Specially Functional Polymeric Materials and Related Technology (Ministry of Education) Shanghai Key Laboratory of Multiphase Materials Chemical Engineering East China University of Science and Technology Shanghai 200237 China State Key Laboratory of Alternate Electrical Power System with Renewable Energy Sources School of New Energy North China Electric Power University Beijing 100096 China i-Lab & CAS Key Laboratory of Nanophotonic Materials and Device Suzhou Institute of Nano-Tech and Nano-Bionics Chinese Academy of Sciences Suzhou 215123 China School of Materials Science and Engineering Xi’an University of Technology Xi’an 710048 China Helmholtz Institute Ulm (HIU) Ulm D89081 Germany Karlsruhe Institute of Technology (KIT) Karlsruhe D76021 Germany

Hard carbons with desirable pore morphologies are the most promising anode materials for sodium-ion batteries, but experience undesirable cycling stability and depressed capacity owing to sluggish reaction kinetics of sodium-related species through or across the carbon layer. Herein, based on closed pore morphology engineering using carbon dioxide physical activation method, the hard carbon composite (SAFe@HC) was prepared by coating a polydopamine capping layer with uniformly distributed iron single atoms on the closed-pore-rich hard carbon, where the introduction SAFe help to expand the layer spacing distance, providing additional channels for solvated Na + diffusion. It is innovatively proposed that SAFe catalysts provide abundant active catalytic sites for accelerating the interfacial desolvation and the phase-transfer kinetics of Na + is lowered by decreasing the sodium ion transport energy barrier, as confirmed by theoretical simulation and various electrochemical demonstration. In addition, the closed pore morphology also enhances the surface area and adsorbs more sodium ions. As a result, the SAFe@HC electrode exhibits a high reversible capacity of 340.7 mAh g −1 and a remarkable rate capacity up to 306.2 mAh g −1 and a high capacity-retention of 96.0 % after 500 cycles at 5C. Decreasing the environmental temperature to 0 °C, an excellent robust electrochemical performance of 172.2 mAh g −1 at 5C, offering promising avenues of single atomic catalysts achieving high-rate hard carbon electrode for sodium-ion batteries.

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