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Taming Electrons in Pt/C Catalysts to Boost the Mesokinetics of Hydrogen Production

Engineering 2022年第7期8卷 124-133页

作者： Wenyao Chen wenzhao fu Xuezhi Duan Bingxu Chen Gang Qian Rui Si Xinggui Zhou Weikang Yuan De Chen State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China Shanghai Synchrotron Radiation Facility Shanghai Institute of Applied PhysicsChinese Academy of SciencesShanghai 201204China Department of Chemical Engineering Norwegian University of Science and TechnologyTrondheim N-7491Norway

Taming the electron transfer across metal–support interfaces appears to be an attractive yet challenging methodology to boost catalytic properties.Herein,we demonstrate a precise engineering strategy for the carbon surface chemistry of Pt/C catalysts—that is,for the electron-withdrawing/donating oxygencontaining groups on the carbon surface—to fine-tune the electrons of the supported metal nanoparticles.Taking the ammonia borane hydrolysis as an example,a combination of density functional theory(DFT)calculations,advanced characterizations,and kinetics and isotopic analyses reveals quantifiable relationships among the carbon surface chemistry,Pt charge state and binding energy,activation entropy/enthalpy,and resultant catalytic activity.After decoupling the influences of other factors,the Pt charge is unprecedentedly identified as an experimentally measurable descriptor of the Pt active site,contributing to a 15-fold increment in the hydrogen generation rate.further incorporating the Pt charge with the number of Pt active sites,a mesokinetics model is proposed for the first time that can individually quantify the contributions of the electronic and geometric properties to precisely predict the catalytic performance.Our results demonstrate a potentially groundbreaking methodology to design and manipulate metal–carbon catalysts with desirable properties.

关键词： Mesokinetics model Catalyst descriptor Pt charge state Carbon surface chemistry Hydrogen generation activity

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Role of surface defects of carbon nanotubes on catalytic performance of barium promoted ruthenium catalyst for ammonia synthesis

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Journal of Energy Chemistry 2020年第2期29卷 79-86页

作者： Yongcheng Ma Guojun Lan wenzhao fu Ying Lai Wenfeng Han Haodong Tang Huazhang Liu Ying Li Institute of Industrial Catalysis Zhejiang University of TechnologyChaowang Road 18Hangzhou 310014ZhejiangChina State Key Laboratory of Chemical Engineering East China University of Science and Technology130 Meilong RoadShanghai 200237China

Carbon nanotubes(CNTs) with abundant surface defects are prepared by a liquid oxidation and thermal annealing method. The defective CNTs-D supported Ba–Ru/CNTs-D catalysts exhibit superior catalytic performance in ammonia synthesis with a TOF be increased up to 0.30 s-1, which is 2.5 times of oxidized CNTs-O supported Ba–Ru/CNTs-O catalysts and 5 times of the Ba–Ru/CNTs. The characterizations by CO chemisorption, transmission electron microscope, Raman, and X-ray photoelectron spectroscopy revealed that the uniformly well dispersed Ru NPs can be stabilized on the defective sites of CNTs-D. The great improvement of the catalytic performance and stability of the Ba–Ru/CNTs-D is contributed to the strong interaction between Ru NPs and surface defect of the CNTs.

关键词： Carbon nanotubes Ruthenium catalyst Defective carbon Ammonia synthesis

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Polyoxometalates-engineered hydrogen generation rate and durability of Pt/CNT catalysts from ammonia borane

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Journal of Energy Chemistry 2020年第2期29卷 142-148页

作者： wenzhao fu Chen Han Dali Li Wenyao Chen Jian Ji Gang Qian Weikang Yuan Xuezhi Duan Xinggui Zhou State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China Department of Chemical Engineering and Applied Chemistry University of TorontoToronto.Ontario M5S 3E5Canada

Heterogeneously catalyzed hydrolytic dehydrogenation of ammonia borane is a remarkable structure sensitive reaction. In this work, a strategy by using polyoxometalates(POMs) as the ligands is proposed to engineer the surface and electronic properties of Pt/CNT catalysts toward the enhanced hydrogen generation rate and durability. Three kinds of POMs, i.e., silicotungstic acid(STA), phosphotungstic acid(PTA)and molybdophosphoric acid(PMA), are comparatively studied, among which the STA shows positive effects on the catalytic activity and durability. A catalyst structure-performance relationship is established by a combination of kinetic and isotopic analyses with multiple characterization techniques, such as HAADF-STEM, EDS, Raman spectroscopy and XPS. It is shown that the STA compared to the other two POMs can increase the Pt binding energy and thus promote the reaction. The insights demonstrated here could open a new avenue for boosting the reaction by employing the POMs as the ligands to engineer the catalyst electronic properties.

关键词： Polyoxometalates Pt/CNT Electronic properties Hydrogen generation Durability

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Active sites of Pt/CNTs nanocatalysts for aerobic base-free oxidation of glycerol

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Green Energy & Environment 2020年第1期5卷 76-82页

作者： Minjian Pan Jingnan Wang wenzhao fu Bingxu Chen Jiaqi Lei Wenyao Chen Xuezhi Duan De Chen Gang Qian Xinggui Zhou State Key Laboratory of Chemical Engineering East China University of Science and Technology130 Meilong RoadShanghai200237China Department of Chemical Engineering Norwegian University of Science and TechnologyTrondheim7491Norway

Understanding the nature of Pt active sites is of great importance for the structure-sensitive base-free oxidation of glycerol. In the present work, the remarkable Pt particle size effects on glycerol conversion and products formation from the oxidation of the primary and the secondary hydroxyl groups are understood by combining the model calculations and DFT calculations, aiming to discriminate the corresponding dominant Pt active sites. The Pt(100) facet is demonstrated to be the dominant active sites for the glycerol conversion and the products formation from the two routes. The insights revealed here could shed new light on fundamental understanding of the Pt particle size effects and then guiding the design and optimization of Pt-catalyzed base-free oxidation of glycerol toward targeted products.

关键词： Base-free oxidation of glycerol Pt/CNTs catalyst Active sites Model calculations DFT calculations

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Formation Mechanism of Reduction Spheroids with Dark Cores in Cretaceous Red Beds in Jiaolai Basin, China

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Open Journal of Geology 2019年第10期9卷 707-710页

作者： Yu Yang wenzhao fu Jifeng Yu Zhenguo Ning Jianjun Cui Qing Li Xuelei Wang Xizhun Zhuo Liaoning Technical University Fuxin China Shandong University of Science and Technology Qingdao China Shandong Institute of Geological Survey Jinan China Institute of Geomechanics Chinese Academy of Geological Sciences Beijing China Laboratory of Paleomagnetism and Tectonic Reconstruction of Ministry of Natural Resources Institute of Geomechanics Chinese Academy of Geological Sciences Beijing China Bureau of Geophysical Prospecting INC. China National Petroleum Corporation Zhuozhou China

Red beds are not entirely red sometimes, in which grey-green spheroids or irregular spots can be found. However, the formation mechanism of grey-green spheroids or irregular spots in red beds is not clear so far. Samples taken from well JK1 in Jiaozhou area of Jiaolai Basin displayed that the reduction spheroids have more Vanadium (V) element, less TFe3O4 and Lead (Pb) element, almost the same content of other elements such as FeO and so on, comparing the red parts of the samples. The existence of organisms can explain the existence of green reductive spheres in the red beds formed under the oxidation environment.

关键词： Red Beds Reduction Spheroids Formation Mechanism Jiaolai Basin Eastern China

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Development of Oligo-GISH kits for efficient detection of chromosomal variants in peanut

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The Crop Journal 2023年第1期11卷 238-246页

作者： Pei Du Liuyang fu Qian Wang Tao Lang Hua Liu Suoyi Han Chenyu Li Bingyan Huang Li Qin Xiaodong Dai wenzhao Dong Xinyou Zhang Henan Academy of Crop Molecular Breeding/State Industrial Innovation Center of Biological Breeding/The Shennong Laboratory/Key Laboratory of Oil Crops in Huang-Huai-Hai Plains Ministry of Agriculture/Henan Provincial Key Laboratory for Oil Crops ImprovementHenan Academy of Agricultural SciencesGraduate T&R Base of Zhengzhou UniversityZhengzhou 450002HenanChina Institute of Biotechnology and Nuclear Technology Sichuan Academy of Agricultural SciencesChengdu 610061SichuanChina

Oligo probe staining is a low-cost and efficient chromosome identification technique.In this study,oligo genomic in situ hybridization(Oligo-GISH)technology was established in peanut.Peanut A and B subgenome-specific interspersed repeat(IR)oligo probe sets were developed based on clustering and electronic localization of tandem repeat sequences in the reference genome of Tifrunner.The OligoGISH kit was then used to perform staining of 15 Arachis species.The A-subgenome probe set stained the chromosomes of A-and E-genome Arachis species,the B-subgenome probe set stained those of B-,F-,K-,and E-genome species,and neither set stained those of H-genome species.These results indicate the relationships among the genomes of these Arachis species.The Oligo-GISH kit was also used for batch staining of the chromosomes of 389 seedlings from the irradiated M1generation,allowing 67 translocation and deletion lines to be identified.Subsequent Oligo-FISH karyotyping,FISH using single-copy probe libraries,and trait investigation identified seven homozygous chromosomal variants from the M3generation and suggested that there may be genes on chromosome 4B controlling seed number per pod.These findings demonstrate that the IR probe sets and method developed in this study can facilitate research on distant hybridization and genetic improvement in peanut.

关键词： Peanut Oligo-GISH Genomic relationship Variants Chromosome identification

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Generation and Display System of Measurement Matrix Based on DMD

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Journal of Beijing Institute of Technology 2018年第4期27卷 493-502页

作者： wenzhao Gu fu Zheng Guangjie Zhai National Space Science Center Chinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100190China

A measurement matrix is the key to sampling and signal reconstruction during the process of compressed sensing.On the basis of digital light processing(DLP)technology,ageneration and display system of measurement matrix based on digital micro-mirror device(DMD)is proposed and well designed.In this system,the generation and controlling of measurement matrix are implemented on a PC,which reduces the hardware requirement to generate a random matrix and overcomes the difficulty of the hardware implementation for the random matrix.It can set up the display number of the measurement matrix,the mode of display and display time according to the requirements from users.The display information can be designed to complete the display of measurement matrix with a better adaptability.The system can be easily embedded into a variety of compressed sensing applications,which can be used to generate and display the corresponding measurement matrice with strong portability.In addition,the DMD of this system will be used as a spatial optical modulator to manipulate near-infrared light in a fast,accurate and efficient way in several applications such as in 3D scanning devices and spectrometers.

关键词： measurement matrix digital micro-mirror device(DMD) compressed sensing Gaussian random matrix

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Micro-size picosecond-duration fast neutron source driven by a laser-plasma wakefield electron accelerator

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High Power Laser Science and Engineering 2022年第5期10卷 57-64页

作者： Yaojun Li Jie Feng wenzhao Wang Junhao Tan Xulei Ge Feng Liu Wenchao Yan Guoqiang Zhang Changbo fu Liming Chen Key Laboratory of Laser Plasma(MoE) School of Physics and AstronomyShanghai Jiao Tong UniversityShanghaiChina IFSA Collaborative Innovation Center Shanghai Jiao Tong UniversityShanghaiChina Shanghai Advanced Research Institute Chinese Academy of SciencesShanghaiChina Key Laboratory of Nuclear Physics and Ion-beam Application(MoE) Institute of Modern PhysicsFudan UniversityShanghaiChina

A pulsed fast neutron source is critical for applications of fast neutron resonance radiography and fast neutron absorption spectroscopy.However,due to the large transversal source size(of the order of mm)and long pulse duration(of the order of ns)of traditional pulsed fast neutron sources,it is difficult to realize high-contrast neutron imaging with high spatial resolution and a fine absorption spectrum.Here,we experimentally present a micro-size ultra-short pulsed neutron source by a table-top laser-plasma wakefield electron accelerator driving a photofission reaction in a thin metal converter.A fast neutron source with source size of approximately 500μm and duration of approximately 36 ps has been driven by a tens of MeV,collimated,micro-size electron beam via a hundred TW laser facility.This micro-size ultra-short pulsed neutron source has the potential to improve the energy resolution of a fast neutron absorption spectrum dozens of times to,for example,approximately 100 eV at 1.65 MeV,which could be of benefit for high-quality fast neutron imaging and deep understanding of the theoretical model of neutron physics.

关键词： fast neutrons high-power laser laser wakefield acceleration photofission reaction

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2020版肺癌多学科团队诊疗中国专家共识解读

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中国肿瘤临床 2022年第4期49卷 163-167页

作者：傅睿吴一龙钟文昭广东省人民医院肿瘤中心广东省医学科学院广东省肺癌研究所广州市510080 华南理工大学医学院

肺癌是一类异质性较高的恶性肿瘤,诊疗有争议、预后不确定的现象屡见不鲜。目前,肺癌的管理呈现个性化、精准化、多学科、综合治疗的发展趋势。基于循证医学的多学科团队(multidisciplinary team,MDT)诊疗融合了最佳证据、专家经验和个... 详细信息

肺癌是一类异质性较高的恶性肿瘤,诊疗有争议、预后不确定的现象屡见不鲜。目前,肺癌的管理呈现个性化、精准化、多学科、综合治疗的发展趋势。基于循证医学的多学科团队(multidisciplinary team,MDT)诊疗融合了最佳证据、专家经验和个人意愿,减少专科医生的选择偏倚,强调对患者诊疗决策的改变,可有效提高患者的临床获益,优化医疗资源使用,提升诊疗的合理性,拓展科研思路,最终使医患双方在多方面获益。为规范中国肺癌MDT诊疗的开展,中国胸部肿瘤研究协作组、中国抗癌协会肺癌专业委员会、中华医学会肿瘤学分会肺癌学组和中国医师协会肿瘤多学科诊疗专业委员会于2020年共同制定了《肺癌多学科团队诊疗中国专家共识》。本文将从MDT的准备、实施、后期、实战应用4个方面对该共识进行解读。

关键词：肺癌多学科团队专家共识诊断治疗

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Redefining the Age of the Cenozoic Shanwang Formation in Shanwang Basin

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Acta Geologica Sinica(English Edition) 2017年第4期91卷 1491-1492页

作者： YU Jifeng ZHAO Xiangguang PANG Xinlong JASON Hilton fu wenzhao ZHAO Xiuli SONG Zhaojun HU Jialiang LU Lei ZHANG Hongjun YANG Ziqun QIAO Wenyan SHI Suo Shandong University of Science and Technology Qingdao 266590 Shandong China Laboratory for Marine Mineral Resources Qingdao National Laboratory for Marine Science and Technology Qingdao 266235 Shandong China Liaoning Technical University Fuxin 123000 Liaoning China University of Birmingham Birmingham B15 2TT U.K.

The Shanwang Basin is a small Cenozoic sedimentary basin located in Linqu county, Shandong province.The Shanwang Formation, especially the diatomaceous shale member, contains diverse and finely preserved flora and fauna fossils （Fig. 1）. Previous paleontological study and radiometric dating show that it was formed in the Miocene. However, on the precise age of the formation, there are such different opinions as Late Miocene, Middle Miocene, Early stage of Middle Miocene, etc.

关键词： data GPTS Redefining the Age of the Cenozoic Shanwang Formation in Shanwang Basin

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