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Nano Research 2024年第11期17卷 9822-9829页

作者： Tianchun Cheng Zhi Wang Shuiyang Fang Hui Jin Chongzhi zhu Shuangyang Zhao Guilin zhuang Qiaoli Chen yihan zhu College of Chemical Engineering and State Key Laboratory Breeding Base of Green Chemical Synthesis Technology Zhejiang University of Technology Hangzhou 310014 China

To ensure the green and sustainable advancement of hydrogen energy, there is a critical need for the development of a cost-effective catalyst to address the sluggish kinetics of water electrolysis under alkaline conditions. An approach to achieve this is by constructing ultrathin Pt shell-structured catalysts that offer enhanced electrocatalytic hydrogen evolution reaction performance through modulation of the inner core while minimizing costs. Herein, an ultrathin Pt shell catalyst with an inner core consisting of a PtNi face-centered cubic and hexagonal-close-packed mixed-phase interface (named PtNi-mix) is synthesized through a pre-synthesis method followed by post-acid etching process. Encouragingly, the PtNi-mix catalyst only requires 12.9 mV overpotential to achieve a current density of 10 mA·cm^(-2) in 1 M KOH, which is much lower than that of the commercial 20 wt.% Pt/C catalyst (71.2 mV). Also, it possesses a high mass activity (7.2 A·mg^(-1)) at an overpotential of 70 mV, which is 9 times higher than that of the commercial 20 wt.% Pt/C catalyst. Additionally, the performance of the PtNi-mix catalyst remains almost unchanged after 10,000 cyclic voltammetry tests, indicating that the catalyst exhibits excellent stability.

关键词： noble metal crystal phase electrocatalysis hydrogen evolution reaction

Tripotassium citrate monohydrate derived carbon nanosheets as a competent assistant to manganese dioxide with remarkable performance in the supercapacitor

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Frontiers of Chemical Science and Engineering 2022年第3期16卷 420-432页

作者： Wenjing Zhang Xiaoxue Yuan Xuehua Yan Mingyu You Hui Jiang Jieyu Miao Yanli Li Wending Zhou yihan zhu Xiaonong Cheng School of Materials Science and Engineering Jiangsu UniversityZhenjiang212013China Institute for Advanced Materials Jiangsu UniversityZhenjiang212013China

Production cost,capacitance,and electrode materials safety are the key factors to be concerned about for *** this work,a type of carbon nanosheets was produced through the carbonization of tripotassium citrate monohydrate and nitric ***,a well-designed manganese dioxide/carbon nanosheets composite was synthesized through hydrothermal *** carbon nanosheets served as the substrate for growing the manganese dioxide,regulating its distribution,and preventing it from inhomogeneous dimensions and severe *** manganese dioxide nanosheets grew vertically on the numerous functional groups generated on the surface of the carbon nanosheets during *** synergistic combination of carbon nanosheets and manganese dioxide tailors the electrochemical performance of the composite,which benefits from the excellent conductivity and stability of carbon *** carbon nanosheets derived from tripotassium citrate monohydrate are conducive to the remarkable performance of manganese dioxide/carbon nanosheets ***,an asymmetric supercapacitor with active carbon as the cathode and manganese dioxide/carbon nanosheets as the anode was assembled,achieving an outstanding energy density of 54.68 Wh·kg^(−1) and remarkable power density of 6399.2 W·kg^(−1) superior to conventional lead-acid *** 10000 charge-discharge cycles,the device retained 75.3%of the initial capacitance,showing good cycle *** assembled asymmetric supercapacitors in series charged for 3 min could power a yellow light emitting diode with an operating voltage of 2 V for 2 *** study may provide valuable insights for applying carbon materials and manganese dioxide in the energy storage field.

关键词： carbon nanosheets manganese dioxide asymmetric supercapacitors energy density power density

Super-conductive silver nanoparticles functioned three-dimensional CuxO foams as a high-pseudocapacitive electrode for flexible asymmetric supercapacitors

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Journal of Materiomics 2021年第1期7卷 156-165页

作者： Hui Jiang Xuehua Yan Le Wang Xiaonong Cheng Jieyu Miao Mingyu You yihan zhu Jianmei Pan School of Materials Science and Engineering Jiangsu UniversityZhenjiang212013JiangsuChina Institute for Advanced Materials Jiangsu UniversityZhenjiang212013JiangsuChina Institute of Green Materials and Metallurgy Jiangsu UniversityZhenjiang212013JiangsuChina

Copper oxide has aroused great concern in energy storage fields due to its properties of high theoretical capacitance,low cost and mild ***,its wide application still remains challenges owing to its poor electrical conductivity and unstable cycling ***-free foam electrodes possess abundant porous structures and high specific surface area,which could get good contact with ***,we demonstrate Ag nanoparticles decorated CuxO nanowires grown spontaneously on copper foam(CF)electrode for asymmetric *** skeleton structure of CF provides large amounts of active sites for the growth of CuxO ***,Ag nanoparticles further decrease the internal resistance and enhance the electrochemical ***/CuxO/CF-40 electrode presents a high area specific capacitance of 1192 mF cm^(-2)at 2 mA cm^(-2)and the influence of surface capacitance-dominated process and diffusion-controlled process are discussed in ***,the energy density of the as-prepared asymmetric supercapacitor(ASC)reaches 46.32 mWh cm^(-2)at a power density of 3.00 mW cm^(-2).A 2V LED is lighted successfully by two ASC in *** work provides a new strategy to prepare low internal resistance and binder-free flexible Ag/CuxO/CF electrode,which demonstrates a good potential application in flexible supercapacitors or other wearable electronic devices.

关键词： Binder-free electrode CuxO nanowire arrays Cu foam Pseudocapacitance contribution Asymmetric supercapacitor

Graphdiyne anchoring to construct highly dense palladium trimer active sites for the selective hydrogenation of acetylene

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Nano Research 2023年第5期16卷 6167-6177页

作者： Rongrong Li Yuxue Yue Xianlang Chen Renqin Chang Jiaxin Zhang Bo Zhao Jieyu Zhang Di Cai yihan zhu Deman Han Jia Zhao Xiaonian Li Engineering Research Center of Recycling and Comprehensive Utilization of Pharmaceutical and Chemical Waste of Zhejiang Province Taizhou UniversityTaizhou 318000China Industrial Catalysis Institute of Zhejiang University of Technology Hangzhou 310014China Research Center of Analysis Measurement of Zhejiang University of Technology Hangzhou 310014China School of Science Zhejiang Sci-Tech UniversityHangzhou 310018China

Semi-hydrogenation of acetylene is of growing interest and popularity but subjects to a major challenge in selective hydrogenation to ***,we report a strategy that uses graphdiyne(GDY)as a carrier to prepare single-cluster catalysts(SCCs),which on average clusters composed of three atoms(denoted as Pd3 trimer)and applied it to the acetylene semihydrogenation in the presence of large amounts of *** on experimental results and systematic quantum chemical research and computational screening,we found that there are multiple active Pd structures on GDY and the Pd3 trimer anchored on GDY is a specific and durable cluster with great potential for accurate and efficient heterogeneous *** synergetic effects between neighboring atoms in Pd trimer guarantee easy desorption of ethylene and the absence of unselective hydride species thereby preventing excessive hydrogenation to generate unwanted byproducts,which is a crucial mechanism for the excellent selectivity of the *** new method for precise synthesis Pd clusters provides accurate ways for designing selective hydrogenation catalysts at the atomic scale.

关键词： Pd cluster catalysts acetylene semi-hydrogenation Pd trimer

Physical regulation of copper catalyst with a hydrophobic promoter for enhancing CO_(2)hydrogenation to methanol

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The Innovation 2023年第4期4卷 67-73页

作者： Hangjie Li Wei Fang Ling-Xiang Wang Yifeng Liu Lujie Liu Tulai Sun Ciqi Liao yihan zhu Liang Wang Feng-Shou Xiao Key Lab of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310028China Key Laboratory of Applied Chemistry of Zhejiang Province Department of ChemistryZhejiang UniversityHangzhou 310028China Center for Electron Microscopy State Key Laboratory Breeding Base of Green Chemistry Synthesis TechnologyCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014China

The hydrogenation of CO_(2)to methanol,which is restricted by water products,requires a selective removal of water from the reaction ***,we show that physically combining hydrophobic polydivinylbenzene with a copper catalyst supported by silica can increase methanol production and CO_(2)*** investigation reveals that the hydrophobic promoter could hinder the oxidation of copper surface by water,maintaining a small fraction of metallic copper species on the copper surface with abundant Cu^(δ+),resulting in high activity for the *** a physically mixed catalyst survives the continuous test for 100 h owing to the thermal stability of the polydivinylbenzene promoter.

关键词： copper methanol hydrogenation

Feasible synthesis of porous h-BN by Mg^(2+)induced lattice dislocations for hydrogen and ammonia storage

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Nano Research 2025年第1期18卷 94-99页

作者： Xiaojia Huang Zihao Wang yihan Kong Li Jiang Baolin Wang Jiangtao Jia Heping Ma Guangshan zhu Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education Northeast Normal UniversityChangchun 130024China School of Chemical Engineering and Technology Xi’an Jiaotong University Xi’an 710049China

Hexagonal boron nitride(h-BN)is a two-dimensional(2D)layered material with a structure similar to graphite and it has potential as a hydrogen and ammonia storage ***,dense packing in the standard h-BN structure limits its surface area and prevents the B and N from being adsorption *** this study,the addition of Mg^(2+)during h-BN synthesis facilitated the growth of lattice dislocations and led to a crosslinked three-dimensional(3D)porous structure.A proposed formation mechanism for porous h-BN was confirmed by several characterization routes,most clearly by high-resolution transmission electron microscopy(HRTEM).Porous Mg/BNs exhibited high H_(2)and NH_(3)uptakes and showed potential for H_(2)and NH_(3)storage.

关键词： hexagonal boron nitride porous material dislocation gas storage

丙烷选择氧化单斜TeMo_5O_(16)催化剂中钒掺杂的作用

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催化学报 2010年第6期31卷 689-694页

作者：董雪朱艺涵李晗陆维敏浙江大学催化研究所浙江省应用化学重点实验室浙江杭州310028

研究了在不同温度下V掺杂的单斜TeMo5O16催化剂上丙烷选择氧化反应性能.结果发现,在保持TeMo5O16相结构基本不变的条件下,V的掺杂提高了催化剂的活性以及丙烯和丙烯醛等脱氢与选择氧化产物的收率.通过程序升温表面反应、拉曼光谱、X射... 详细信息

研究了在不同温度下V掺杂的单斜TeMo5O16催化剂上丙烷选择氧化反应性能.结果发现,在保持TeMo5O16相结构基本不变的条件下,V的掺杂提高了催化剂的活性以及丙烯和丙烯醛等脱氢与选择氧化产物的收率.通过程序升温表面反应、拉曼光谱、X射线光电子能谱、X射线衍射、程序升温还原和热重分析等手段对其原因进行了探讨.结果表明,V的掺杂引起催化剂表面金属–氧键发生变化,提高了表面氧化还原中心的活性,增加了酸性中心数目,从而提高了催化剂活化丙烷能力.同时,较高的V掺杂量可以提高催化剂体相中晶格氧参与氧化还原的能力.

关键词：丙烷选择氧化钼碲复合氧化物钒掺杂

四维扫描透射电子显微镜技术:从材料微观结构到物性分析

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物理化学学报 2023年第3期39卷 43-57页

作者：冯启龙朱翀之盛冠孙土来李永合朱艺涵浙江工业大学化学工程学院前沿交叉科学研究院电子显微镜中心(分析测试中心)杭州310014

扫描透射电子显微镜(Scanning transmission electron microscopy,STEM)目前已经达到了原子级分辨率,并且由于其具有灵活的多通道成像能力以及强大的与谱学分析相结合的特点,因此在材料科学、生命科学等领域展现出强大的微尺度表征能力... 详细信息

扫描透射电子显微镜(Scanning transmission electron microscopy,STEM)目前已经达到了原子级分辨率,并且由于其具有灵活的多通道成像能力以及强大的与谱学分析相结合的特点,因此在材料科学、生命科学等领域展现出强大的微尺度表征能力。但传统STEM的探测器受单像素积分式探测机制的限制,使其只能收集特定角度的散射电子,这导致不仅丢失了散射电子的角分辨信息,还降低了入射电子的剂量效率,因此迫切需要发展全新成像技术来实现高通量、高电子剂量效率成像。近年来,电子探测技术和分区或像素化探测器的研发联合计算机运算、存储能力的大幅提高,推动了四维扫描透射电子显微镜技术(Four-dimensional scanning transmission electron microscopy,4D-STEM)的蓬勃发展,并为最大化、最高效挖掘散射电子信息带来希望。在采集4D-STEM数据时,会聚电子束在样品平面上进行二维扫描,与此同时使用一块具有高帧速、高动态范围以及高信噪比的像素化阵列式探测器在远场收集二维的衍射数据。因为这些衍射数据是角度解析的,所以既可以用来进行常规的STEM成像,也可以用来实现前沿的相位衬度成像。例如利用电子叠层重构(Ptychography)技术通过在不同空间位置测量的一系列衍射花样来重建样品物函数。此外,4D-STEM技术还可以被进一步挖掘从而获得更多关于材料内部结构的信息,这为材料的多尺度表征带来机会。本文从4D-STEM技术原理介绍开始,总结了4D-STEM技术从材料微观结构到物性分析方面的一系列应用。具体而言,内容包含了虚拟探测器成像、微区电磁场测量、微区晶体取向测量、微区应变分布测量以及材料局域厚度测量等材料微尺度表征方面的原理和应用。除此之外,利用4D-STEM数据实现的电子叠层重构成像技术因为具有较高的散射电子利用效率,所以在低电子剂量领域展现出极大的应用潜力,因此本文还对4D-STEM技术在低电子剂量领域的应用进行了探讨与展望。总而言之,随着电子探测器以及4D-STEM数据后处理分析软件的快速发展,相信新颖的4D-STEM技术最终将彻底取代传统的扫描透射电子显微镜。

关键词：扫描透射电子显微镜电磁场分布叠层成像晶体取向应变分布低剂量成像

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利用价键和周期密度泛函理论研究MoVTeNbO复合氧化物(M1相)催化剂的活性中心

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催化学报 2010年第10期31卷 1286-1292页

作者：朱艺涵陆维敏董雪王阳马飞浙江大学催化研究所浙江省应用化学重点实验室浙江杭州310028

采用价键分析和周期密度泛函理论相结合的方法,研究了具有M1晶相结构的MoVTeNbO复合氧化物催化剂中各活性中心的d电子性质.通过分析各活性中心配对出现的d电子和氧缺位的可能分布,得到了最可能高效完成丙烷选择氧化反应的M-M-Te(M=Mo或V... 详细信息

采用价键分析和周期密度泛函理论相结合的方法,研究了具有M1晶相结构的MoVTeNbO复合氧化物催化剂中各活性中心的d电子性质.通过分析各活性中心配对出现的d电子和氧缺位的可能分布,得到了最可能高效完成丙烷选择氧化反应的M-M-Te(M=Mo或V)活性中心组合.此外,根据各活性中心对骨架稳定的贡献,说明了稳定的M1相骨架主要来自MoO6八面体中赤道面上的强共价Mo–O键,而VO6八面体的贡献较小.通常被认为稳定M1相的Nb物种主要以离子键的形式存在于五边形孔道中,因而Nb5+作为一种模板离子,诱导五边形孔道乃至M1晶相结构的生成.

关键词：丙烷选择氧化钼钒碲铌复合氧化物价键密度泛函理论活性中心

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Mo基复合金属氧化物催化丙烷氧化制丙烯醛

石油化工 2006年第8期35卷 730-734页

作者：宋振陆维敏朱艺涵 Achim Fischer 浙江大学催化研究所浙江杭州310028 德固赛股份公司

制备了Mo基复合金属氧化物(MoMxOn,M=C r,Co,Zn,Mn,Nb,Ce)催化剂,评价了不同金属含量的MoMxOn催化剂在不同温度下对丙烷选择性氧化制备丙烯醛反应的催化性能。在所研究的各种MoMxOn催化剂中,MoCo0.1On催化剂在773 K时的催化性能最佳,丙... 详细信息

制备了Mo基复合金属氧化物(MoMxOn,M=C r,Co,Zn,Mn,Nb,Ce)催化剂,评价了不同金属含量的MoMxOn催化剂在不同温度下对丙烷选择性氧化制备丙烯醛反应的催化性能。在所研究的各种MoMxOn催化剂中,MoCo0.1On催化剂在773 K时的催化性能最佳,丙烯醛的收率为9.3%。Raman光谱和X射线衍射表征结果表明,除MoNbxOn催化剂外,其他各种MoMxOn催化剂中的主要物相是MoO3,说明MoO3可能对催化活性起重要作用。增加Co含量使MoO3衍射峰的相对强度发生改变,可能是引起MoCoxOn催化剂氧化性能下降的原因。

关键词：丙烷丙烯醛钼复合金属氧化物催化剂选择性氧化