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Acetic acid-assisted mild dealloying of fine CuPd nanoalloys achieving compressive strain toward high-efficiency oxygen reduction and ethanol oxidation electrocatalysis

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Carbon Energy 2023年第7期5卷 112-120页

作者： Danye Liu Yu Zhang Hui Liu Peng Rao Lin Xu Dong Chen Xinlong Tian Jun Yang State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijingChina State Key Laboratory of Marine Resource Utilization in South China Sea Hainan Provincial Key Lab of Fine ChemistrySchool of Chemical Engineering and TechnologyHainan UniversityHaikouChina Jiangsu Key Laboratory of New Power Batteries School of Chemistry and Materials ScienceJiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsNanjing Normal UniversityNanjingChina Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijingChina Nanjing IPE Institute of Green Manufacturing Industry NanjingJiangsuChina

Dealloying by which the transition metal is partially or completely leached from an alloy precursor is an effective way to optimize the fundamental effects for further enhancing the electrocatalysis of a ***,to address the deficiencies associated with the commonly used dealloying methods,for example,electrochemical and sulfuric acid/nitric acid treatment,we report an acetic acid-assisted mild strategy to dealloy Cu atoms from the outer surface layers of CuPd alloy nanoparticles to achieve high-efficiency electrocatalysis for oxygen reduction and ethanol oxidation in an alkaline *** leaching of Cu atoms by acetic acid exerts an additional compressive strain effect on the surface layers and exposes more active Pd atoms,which is beneficial for boosting the catalytic performance of a dealloyed catalyst for the oxygen reduction reaction(ORR)and the ethanol oxidation reaction(EOR).In particular,for ORR,the CuPd nanoparticles with a Pd/Cu molar ratio of 2:1 after acetic dealloying show a half-wave potential of 0.912 V(***)and a mass activity of 0.213 AmgPd^(-1) at 0.9 V,respectively,while for EOR,the same dealloyed sample has a mass activity and a specific activity of 8.4 Amg^(-1) and 8.23 mA cm^(-2),respectively,much better than their dealloyed counterparts at other temperatures and commercial Pd/C as well as a Pt/C catalyst.

关键词： compressive strain effect dealloying electrocatalysis ethanol oxidation reaction oxygen reduction reaction

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生物启发和生物工程核酸药物载体

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Science China Materials 2024年第8期67卷 2393-2413页

作者：左嘉敏卢治国郭京赵睿琛张田露王朝霞袁云邓健文袁俊亮张欣 State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100049China Department of Neurology Peking University Sixth HospitalPeking University Institute of Mental HealthBeijing 100191China Department of Neurology Peking University First HospitalBeijing 100034China Beijing Key Laboratory of Neurovascular Disease Discovery Beijing 100034China Key Laboratory of Biopharmaceutical Preparation and Delivery Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China

核酸药物具有直接作用于致病基因的优势,在治疗各种疾病方面具有巨大潜力.然而,由于核酸药物需要克服多重生理障碍才能到达靶点,因此在实际应用中面临诸多困难和挑战.为了提高核酸药物的稳定性和递送效率,研究人员开始利用生物工程化和... 详细信息

核酸药物具有直接作用于致病基因的优势,在治疗各种疾病方面具有巨大潜力.然而,由于核酸药物需要克服多重生理障碍才能到达靶点,因此在实际应用中面临诸多困难和挑战.为了提高核酸药物的稳定性和递送效率,研究人员开始利用生物工程化和生物启发材料所具有的内源性递送生物大分子的能力来递送核酸药物.本文重点介绍核酸药物递送过程中需要克服的生物障碍,以及生物工程和生物启发材料在核酸药物递送中的优势和应用.通过利用这些先进的生物材料,研究人员有望提高核酸药物的疗效,为疾病治疗提供新的解决方案.

关键词：生物工程药物递送生理障碍生物启发致病基因生物大分子工程化疾病治疗

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In-situ synthesis of N, S co-doped hollow carbon microspheres for efficient catalytic oxidation of organic contaminants

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Chinese Chemical Letters 2022年第3期33卷 1298-1302页

作者： Yongbing Xie Ya Liu Yujie Yao Yanchun Shi Binran Zhao Yuxian Wang State Key Laboratory of Vanadium and Titanium Resources Comprehensive Utilization Panzhihua 617000China CAS Key Laboratory of Green Process&Engineering Beijing Engineering Research Center of Process Pollution ControlInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China State Key Laboratory of Heavy Oil Processing State Key Laboratory of Petroleum Pollution ControlChina University of Petroleum-BeijingBeijing 102249China School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaideSA 5005Australia School of Chemical Engineering Northwest UniversityXi'an 710069China

Metal-free heteroatom doped nanocarbons are promising alternatives to the metal-based materials in catalytic ozonation for destruction of aqueous organic contaminants. In this study, N, S co-doped hollow carbon microspheres (NSCs) were synthesized from the polymerization products during persulfate wet air oxidation of benzothiazole. The contents of doped N and S as well as the structural stability were maneuvered by adjusting the subsequent N_(2)-annealing temperature. Compared with the prevailing single-walled carbon nanotubes, the N_(2)-annealed NSCs demonstrated a higher catalytic ozonation activity for benzimidazole degradation. According to the quantitative structure-activity relationship (QSAR) analysis, the synergistic effect between the graphitic N and the thiophene-S which redistributed the charge distribution of the carbon basal plane contributed to the activity enhancement of the N_(2)-annealed NSCs. Additionally, the hollow structure within the microspheres served as the microreactor to boost the mass transfer and reaction kinetics via the nanoconfinement effects. Quenching and electron paramagnetic resonance (EPR) tests revealed that benzimidazole degradation was dominated by the produced singlet oxygen (^(1)O_(2)) species, while hydroxyl radicals (^(·)OH) were also generated and participated. This study puts forward a novel strategy for synthesis of heteroatom-doped nanocarbons and sheds a light on the relationship between the active sites on the doped nanocarbons and the catalytic performance.

关键词： Metal-free catalysis Hollow carbon microspheres N,S co-doping Catalytic ozonation Singlet oxygen(1O_(2))

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EM-DETR: Efficient Multi-scale DETR for Gas Leak Detection Based on Infrared Imaging

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IEEE Sensors Journal 2025年第11期25卷 20538-20546页

作者： Wang, Qi Zhu, Shilin Lu, Zhenlin Sun, Yunlong Qian, Yizhuo Hebei Key Laboratory of Micro-Nano Precision Optical Sensing and Measurement Technology Qinhuangdao066004 China Northeastern University State Key Laboratory of Synthetical Automation for Process Industries Shenyang110819 China Northeastern University College of Information Science and Engineering Shenyang110819 China Beijing Institute of Microelectronics Technology Beijin100076 China

Industrial gases play a crucial role in modern industrial production. However, many industrial gases are only visible in the infrared spectrum. Therefore, using infrared camera for gas leak detection is essential for the normal operation of production lines and the safety of personnel. Existing automatic leak detection algorithms based on convolutional neural networks often involve numerous handcrafted feature components, resulting in complex model architectures, with hyperparameter selection significantly impacting model performance. To address these issues, we propose an efficient and high-performance end-to-end object detection network, the Efficient Multi-scale Detection Transformer (EM-DETR), for automatic gas leak detection. To reduce model computational overhead, we design a new efficient encoder. Additionally, to handle leaks of varying ranges due to gas dispersion, we implement bidirectional fusion of multi-scale features to capture granularity information of gases at different scales. Finally, based on the similar unified distribution of gas leak images, we introduce a pre-auxiliary loss to adjust the learnable object queries initialized. Experimental results demonstrate that the EM-DETR R50/R101 outperforms previous methods, achieving 40.7%/43.2% AP on gas leak infrared image datasets with minimal parameters and computational resources, providing a superior solution for automatic gas leak detection using infrared camera. © 2001-2012 IEEE.

关键词： Convolutional neural networks

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Manipulating d-d orbital hybridization induced by Mo-doped Co_(9)S_(8) nanorod arrays for high-efficiency water electrolysis

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Journal of Energy Chemistry 2024年第6期93卷 592-600,I0015页

作者： Xue Zhou Jing Li Guangyao Zhou Weiran Huang Yucan Zhang Jun Yang Huan Pang Mingyi Zhang Dongmei Sun Yawen Tang Lin Xu Jiangsu Key Laboratory of New Power Batteries Jiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023JiangsuChina 'College of Science Jinling Institute of TechnologyNanjing 211169JiangsuChina State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Nanjing IPE Institute of Green Manufacturing Industry Nanjing 211100JiangsuChina School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225009JiangsuChina Key Laboratory for Photonic and Electronic Bandgap Materials Ministry of EducationSchool of Physics and Electronic EngineeringHarbin Normal UniversityHarbin 150025HeilongjiangChina

Precisely refining the electronic structure of electrocatalysts represents a powerful approach to further optimize the electrocatalytic ***,we demonstrate an ingenious d-d orbital hybridization concept to construct Mo-doped Co_(9)S_(8) nanorod arrays aligned on carbon cloth(CC)substrate(abbreviated as Mo-Co_(9)S_(8)@CC hereafter)as a high-efficiency bifunctional electrocatalyst toward water *** has experimentally and theoretically validated that the 4d-3d orbital coupling between Mo dopant and Co site can effectively optimize the H_(2)O activation energy and lower H^(*)adsorption energy barrier,thereby leading to enhanced hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)*** to the unique electronic and geometrical advantages,the optimized Mo-Co_(9)S_(8)@CC with appropriate Mo content exhibits outstanding bifunctional performance in alkaline solution,with the overpotentials of 75 and 234 mV for the delivery of a current density of 10 mA cm^(-2),small Tafel slopes of 53.8 and 39.9 mV dec~(-1)and long-term stabilities for at least 32 and 30 h for HER and OER,*** impressively,a water splitting electrolylzer assembled by the self-supported Mo-Co_(9)S_(8)@CC electrode requires a low cell voltage of 1.53 V at 10 mA cm^(-2)and shows excellent stability and splendid reversibility,demonstrating a huge potential for affordable and scalable electrochemical H_(2) *** innovational orbital hybridization strategy for electronic regulation herein provides an inspirable avenue for developing progressive electrocatalysts toward new energy systems.

关键词： d-d orbital hybridization Transition metal sulfides Nanorods arrays Water electrolysis

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Assembling molybdenum-doped platinum clusters into a coral-like nanostructure for highly enhanced oxygen reduction

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eScience 2024年第1期4卷 123-131页

作者： Linwei Zheng Mang Niu Tiantian Zeng Xiaohang Ge Yanrui Wang Chun Xian Guo Weiyong Yuan Dapeng Cao Lian Ying Zhang Chang Ming Li Institute of Materials for Energy and Environment Institute of Biochemical EngineeringCollege of Materials Science and EngineeringQingdao UniversityQingdao 266071China Institute for Materials Science and Devices School of Materials Science and EngineeringSuzhou University of Science and TechnologySuzhou 215011PR China Ningbo Research Institute Zhejiang UniversityNingbo 315100China State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China

Regulating the electronic and geometric structures of electrocatalysts is an effective strategy to boost their catalytic ***,a coral-like nanostructure is assembled with Mo-doped Pt clusters to form a highly active catalyst toward the oxygen reduction reaction(ORR).The advantages of a Mo-doped porous skeleton,grain boundaries,and MoOx species on the Pt cluster surfaces synergistically boost the electrocatalytic *** unique architecture delivers 3.5-and 2.8-fold higher mass and specific activities,respectively,than commercial Pt/*** functional theory calculations reveal that the Mo-doped Pt clusters have an optimized Pt–O bond length of 2.110Å,which weakens the adsorption energy of the intermediate O*to yield great ORR ***,the catalyst shows a decay in the half-wave potential of only 8 mV after 10,000 cycles of accelerated durability *** high stability arises from the increased dissociation energy of Pt atoms and the stable architecture of the coral-like structure of clusters.

关键词： Pt clusters Mo doping Porous structure Pt-O bond Oxygen reduction reaction

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Bridging buried interface enable 24.67%-efficiency doctor-bladed perovskite solar cells in ambient condition

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Nano Research 2024年第9期17卷 8068-8076页

作者： Jianhui Chang Erming Feng Xiangxiang Feng Hengyue Li Yang Ding Caoyu Long Siyuan Lu Haixia Zhu Wen Deng Jiayan Shi Yingguo Yang Si Xiao Yongbo Yuan Junliang Yang Hunan Key Laboratory for Super-microstructure and Ultrafast Process School of PhysicsCentral South UniversityChangsha 410083China Hunan Key Laboratory of Nanophotonics and Devices School of PhysicsCentral South UniversityChangsha 410083China Textile and Fashion Collage Hunan Institute of EngineeringXiangtan 411101China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China State Key Laboratory of Powder Metallurgy Central South UniversityChangsha 410083China

Scalable deposition of high-efficiency perovskite solar cells(PSCs)is critical to accelerating their commercial ***,a significant number of defects are distributed at the buried interface of perovskite film fabricated by scalable deposition,exhibiting much negative influence on the efficiency and stability of ***,2-(N-morpholino)ethanesulfonic acid potassium salt(MESK)is incorporated as the bridging layer between the tin oxide(SnO_(2))electron transport layer(ETL)and the perovskite film deposited via scalable two-step doctor *** experiment and simulation results demonstrate that MESK can passivate the trap states of Sn suspension bonds,thereby enhancing the charge extraction and transport of the SnO_(2)***,the strong interaction with uncoordinated Pb ions can modulate the crystal growth and crystallographic orientation of perovskite film and passivate buried *** employing MESK interface bridging,PSCs fabricated via scalable doctor blading in ambient condition achieve a power conversion efficiency(PCE)of 24.67%,which is one of the highest PCEs for doctor-bladed PSCs,and PSC modules with an active area of 11.35 cm^(2)achieve a PCE of 19.45%.Furthermore,PSCs exhibit excellent long-term stability,and the unpackaged target device with a storage of 1680 h in ambient condition(25℃and humidity of 30%relative humidity(RH))can maintain more than 90%of the initial *** research provides a strategy for constructing a high-performance interface bridge between SnO_(2)ETL and perovskite film,and achieving efficient and stable large-area PSCs and modules fabricated via scalable doctor-blading process in ambient condition.

关键词： perovskite solar cells doctor blading buried interface defect passivation orientation regulation

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Pt confined in Sn-ECNU-46 zeolite for efficient alkane dehydrogenation

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Chinese Journal of Structural Chemistry 2024年第4期43卷 15-23页

作者： Naihong Wang Longkang Zhang Yejun Guan Peng Wu Hao Xu Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular Engineering East China Normal UniversityShanghai200062China State Key Laboratory of Petroleum Molecular&Process Engineering SKLPMPE Sinopec Research Institute of Petroleum Processing Co.LTD.Beijing100083China East China Normal University Shanghai200062China

Highly dispersed and stable Pt-based catalysts play a crucial role in constructing efficient catalytic systems for alkane *** this study,a novel bimetallic Pt-Sn catalyst confined in extra-large-pore ECNU-46 zeolite(denoted as Pt/Sn-ECNU-46)is prepared by *** open-site framework Sn species((SiO)_(3)Sn-OH)serve as anchors to interact with Pt species,favoring the high dispersion of *** the other hand,the framework Sn species act as the second metal to regulate the geometrical and electronic environment of Pt species,thus suppressing their ***/Sn-ECNU-46 achieves a good performance in propane dehy-drogenation(PDH)reaction with high initial propane conversion(46%)and propylene selectivity(>99%)as well as regeneration *** addition,Pt/Sn-ECNU-46 is also active in the dehydrogenation of *** study explores the application of extra-large-pore zeolite as support in constructing metal-confined catalysts for alkane dehydrogenation.

关键词： Alkane dehydrogenation Heteroatom-containing zeolite Zeolite confined catalyst Pt-based catalyst

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Multi-site observation of large-scale eddies in the surface layer of the Loess Plateau

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Science China Earth Sciences 2023年第4期66卷 871-881页

作者： Jinbei CHEN Xiaowen CHEN Wei JIA Ye YU Suping ZHAO Key Laboratory of Land Surface Process and Climate Change in Cold and Arid Regions Northwest Institute of Eco-Environment and ResourcesChinese Academy of SciencesLanzhou 730000China Key Laboratory of Middle Atmosphere and Global Environment Observation(LAGEO) Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China Mechanical Engineering Department Pennsylvania State UniversityState College 16802USA

This article aims to build a theory of atmospheric boundary layer turbulence under complex conditions. To achieve this goal, we constructed a multi-site observation and analysis method of atmospheric turbulence based on related *** method first requires verification for the ergodicity of the full-scale observation of surface-layer turbulence, which proves that eddies within a scale of 60 min during a four-site observation can easily meet ergodicity. Meanwhile, by applying the second-order structure function for the horizontal wind speed turbulence of a single site and upstream and downstream points, we verified the ergodicity of the turbulence observation. Comparing the turbulence spectrum to the second-order structure function for the horizontal wind speed from the four-site observation, a relatively high accordance was observed, proving the reasonability of the multi-site observation. Moreover, compared to the single-site observation, the four-site observation can improve the estimation accuracy of the surface-layer turbulence spectrum and vertical turbulent flux. As a result, we can describe the threedimensional structure of turbulence more accurately and comprehensively by combining analytical data from single-site and four-site observations. In summary, the multi-site turbulence observation method shows that the horizontal and vertical wind turbulence of the Baimiao plateau has a typical structure of a turbulence spectrum with clear spectral gaps. The result is in accordance with the scale of the turbulence spectral gaps obtained from the 6 h data. The horizontal wind speed is under the influence of the terrain, so its spectrum of large-scale eddies has higher fluctuations, but its spectral gaps can still be clearly distinguished. Although the spectral gaps of the temperature spectrum are not distinguishable, they still have the same scale as the spectral gap of the vertical and horizontal turbulence spectrum. Moreover, the temperature spectrum poss

关键词： Larger-scale eddy Complex condition Ergodicity of turbulence observation Structure function Turbulence spectrum

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Effects of zinc on χ-Fe_(5)C_(2) for carbon dioxide hydrogenation to olefins:Insights from experimental and density function theory calculations

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Chinese Journal of Chemical engineering 2023年第2期54卷 206-214页

作者： Xianglin Liu Minjie Xu Chenxi Cao Zixu Yang Jing Xu State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China Maoming Branch R&D Institute SINOPECMaoming 525000China Key Laboratory of Smart Manufacturing in Energy Chemical Process Ministry of EducationEast China University of Science and TechnologyShanghai 200237China

Production of light olefins from CO_(2), the primary greenhouse gases, is of great importance to mitigate the adverse effects of CO_(2) emission on environment and to supply the value-added products from nonpetroleum resource. However, development of robust catalyst with controllable selectivity and stability remains a challenge. Herein, we report that Zn-promoted Fe catalyst can boost the stable and selective production of light olefins from CO_(2). Specifically, the Zn-promoted Fe exhibits a highly stable activity and olefin selectivity over 200 h time-on-stream compared to the unpromoted Fe catalyst, primarily owing to the preservation of active χ-Fe_(5)C_(2) phase. Structural characterizations of the spent catalysts suggest that Zn substantially regulates the content of iron carbide on the surface and suppresses the reoxidation of bulk iron carbide during the reaction. DFT calculations confirm that adsorption of surface carbon atoms and graphene-like carbonaceous species are not thermochemically favored on Zn-promoted Fe catalyst. Carbon deposition by CAC coupling reactions of two surface carbon atoms and dehydrogenation of CH intermediate are also inhibited. Furthermore, the effects of Zn on antioxidation of iron carbide were also investigated. Zn favored the hydrogenation of surface adsorbed oxygen atoms to H_(2)O and the desorption of H_(2)O, which reduces the possibility of surface carbide being oxidized by the chemisorbed oxygen.

关键词： Reaction engineering χ-Fe_(5)C_(2) Zn promoter Carbon dioxide Hydrogenation Density function theory

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