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Cobalt phthalocyanine promoted copper catalysts toward enhanced electro reduction of CO_(2)to C_(2):Synergistic catalysis or tandem catalysis?

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Journal of Energy Chemistry 2024年第5期92卷 499-507页

作者： Yan Luo Jun Yang Jundi Qin kanghua miao Dong Xiang Aidar Kuchkaev Dmitry Yakhvarov Chuansheng Hu Xiongwu Kang New Energy Research Institute School of Environment and EnergySouth China University of TechnologyHigher Education Mega CenterGuangzhou 510006GuangdongChina Guangdong University of Petrochemical Technology School of Chemical EngineeringMaoming 525000GuangdongChina Arbuzov Institute of Organic and Physical Chemistry FRC Kazan Scientific Center of RASArbuzov Street 8Kazan 420088Russian Federation National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029AnhuiChina

The activity and selectivity of electrocatalytic CO_(2)reduction reaction(CO_(2)RR)to C_(2)products on metal catalysts can be regulated by molecular ***,the mechanism behind it remains elusive and ***,copper nanowires(Cu NWs)were fabricated and decorated with cobalt phthalocyanine(CoPc).The electronic interaction between the Cu NWs,CoPc,CO_(2) and CO_(2)RR intermediates were explored by density functional theory(DFT)*** was found that the selectivity and activity of CO_(2)RR towards C_(2)products on Cu NWs were considerably enhanced from 35.2%to 69.9%by surface decoration of *** calculations revealed that CO_(2)RR can proceed in the interphase between Cu substrate and CoPc,and the CO_(2)RR intermediates could synergistically bond with both Cu and Co metal centre in CuNWs-CoPc,which favours the adsorption of CO_(2),CO and CO_(2)RR intermediates,thus reducing the free energy for CO-COcoupling towards C_(2)*** synergistic interaction was further extended to phthalocyanine(Pc)and other metal phthalocyanine derivatives(MPc),where a relatively weaker synergistic interaction of COintermediates with MPc and Cu substrate and only a slight enhancement of CO_(2)RR towards C_(2) products were *** study demonstrates a synergistic catalysis pathway for CO_(2)RR,a novel perspective in interpreting the role of CoPc in enhancing the activity and selectivity of CO_(2)RR on Cu NWs,in contrast to the conventional tandem catalysis mechanism.

关键词： CO_(2)reduction reaction Raman spectroscopy Synergistic catalysis DFT calculation

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胺功能化的铜催化剂:氢键介导的电化学CO_(2)还原为C_(2)产物以及优越的可充电Zn-CO_(2)电池性能

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物理化学学报 2024年第8期40卷 43-46页

作者：项东李坤振苗康华龙冉熊宇杰康雄武华南理工大学新能源研究所环境与能源学院广州510006 中国科学技术大学合肥微尺度物质科学国家研究中心化学与材料科学学院合肥230026

有机分子功能化是一种有前景的策略,用于调控电化学CO_(2)还原反应(eCO_(2)RR)的C_(2+)产物选择性和活性。然而,我们对于电化学CO_(2)还原调控机制的分子水平理解仍然不够清晰。在本文中,我们成功制备了铜纳米颗粒,并使用一系列胺类衍生... 详细信息

有机分子功能化是一种有前景的策略,用于调控电化学CO_(2)还原反应(eCO_(2)RR)的C_(2+)产物选择性和活性。然而,我们对于电化学CO_(2)还原调控机制的分子水平理解仍然不够清晰。在本文中,我们成功制备了铜纳米颗粒,并使用一系列胺类衍生物(如十六胺(HAD)、N-甲基十六胺(N-MHDA)、十六烷基二甲胺(HDDMA)和十六酰胺(PMM))对其进行功能化,以系统地研究胺表面活性剂分子结构对eCO_(2)RR选择性和活性的影响。结果表明,HDA的功能化可以将C_(2)产物和C_(2)H_(4)的法拉第效率(FE)提高至73.5%和46.4%,并且在−0.9 V ***(可逆氢电极)电位下,C_(2)产物的分电流密度为131.4 mA·cm^(−2)。理论研究发现,HDA通过与CO_(2)和eCO_(2)RR中间体之间的氢键相互作用,富集了^(*)CO_(2)、^(*)CO和其他反应中间体,降低了CO―CHO耦合反应的动力学能垒,从而促进了eCO_(2)RR向C_(2)产物的转化。当胺基的H原子被甲基取代后,氢键相互作用减弱,竞争的析氢反应加剧。PMM通过Cu―O键与Cu表面发生键合,而不是通过Cu―N键,导致Cu-PMM更倾向于产乙醇。原位拉曼光谱显示,在Cu-HDA表面,CO主要吸附在Cu的顶位吸附位点上,与在Cu表面上的桥式吸附不同,这可能是因为前者表面对CO的富集引发了CO的吸附构型变化。HDA功能化还提高了Cu催化剂的表面pH。基于Cu-HDA组装的可充电Zn-CO_(2)电池在放电电流密度为16 mA∙cm^(−2)时,最大功率密度为6.48 mW∙cm^(−2),并具有长达60 h的良好充放电稳定性。本研究的重点在于通过在分子水平上调节Cu基材料的CO_(2)RR活性和选择性,促进CO_(2)-C_(2)的转化,这可能为提高C_(2)产物的产率提供新的见解。

关键词：二氧化碳还原 CO―CHO耦合有机分子功能化原位拉曼 C_(2)产物 Zn-CO_(2)电池

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Three New Compounds Based on 4,4＇-Azo-l,2,4-triazol-5-one： Synthesis, Crystal Structure and Thermal Properties

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Chemical Research in Chinese Universities 2016年第5期32卷 812-817页

作者： GUO Jiajia HUANG Jie SONG Jirong miao kanghua CAO Wenli School of Chemical Engineering Shaanxi Key Laboratory of Physico-Inorganie Chemistry Northwest University Xi 'an 710069 P. R. China Consewation Technology Department the Palace Museum Beo'ing 100009 P R. China

A series of guanidine salts of 4,4＇-azo-l,2,4-triazol-5-one with guanidine（1）, aminoguanidine（2）, diaminoguanidine（3） and triaminoguanidine（4） was prepared. Compounds 2--4 were characterized by infrared（IR） spectroscopy, elemental analysis and single-crystal X-ray diffraction. Thermal decomposition processes of compounds 1--4 were investigated by differential scanning calorimetry（DSC）, and all the compounds showed good thermal stability up to 190 ℃. Moreover, these four guanidine salts are more unstable with the increasing number of amino groups. Thermal stability parameters（Te,0 and Tb）and thermodynamic functions（△S≠, △H≠ and △G≠） for compounds 1-4 were calculated. The constant-volume combustion heats（AcU） for compounds 2--4 were determined and tended to increase with the increase of the number of amino groups. The calculated standard molar enthalpies of forma- tion（△ρH0m） of compounds 2-4 are -541.04, -178.67 and-83.08 kJ/mol, respectively. The impact sensitivities results indicate that these four energetic salts are less sensitive than 1,3,5-trinitrotriazacyccohexane（RDX） and 1,3,5,7- tetranitrotetraqza-cyclo-octane（HMX）.

关键词： 4,4'-Azo-1,2,4-triazol-5-one High-nitrogen energetic compound X-Ray diffraction Thermal property

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Enhanced Catalytic Activity of Metal Nanomaterials by Surface and Interface Engineering

Enhanced Catalytic Activity of Metal Nanomaterials by Surfac...

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2019第四届中国能源材料化学研讨会

作者：康雄武 Fengqi Zhang Zhiwei Guo kanghua miao Lin Huang 华南理工大学 School of Environment and Energy South China University of Technology

＜正＞It is desirable to develop catalyst of high performance and low cost for the commercialization of direct formic acid/methanol fuel cells and industrial production of organic feed *** we prepared a series of PdCu and PdRu nanoparticles and both the size effect and the metal-support interactions are investigated in details.

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Enhanced Catalytic Activity of Metal Nanomaterials by Surface and Interface Engineering

Enhanced Catalytic Activity of Metal Nanomaterials by Surfac...

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中国化学会2019能源材料和缺陷化学研讨会

作者： Xiongwu Kang kanghua miao Zhiwei Guo Fengqi Zhang Lin Huang School of Environment and Energy South China University of Technology

It is desirable to develop catalyst of high performance and low cost for the commercialization of direct formic acid/methanol fuel cells and industrial production of organic feed stocks. Here we prepared a series of PdCu nanoparticles and the size effect on the metal-support interactions are investigated in details. The interaction of PdCu alloy nanoparticles with CeO2 support induces compressive strain, down-shift of the d-band center, reduced CO binding energy and augmentation of PdO content for PdCu nanoparticles. It is concluded that the synergy of compressive strain, enhanced Pd O and oxygen vacancy remarkably promotes the catalytic performance of PdCu towards electrooxidation of formic acid, while electrooxidation of methanol on PdCu is promoted only by the oxygen vacancy. It is also noted that the surface functionalization of Ru nanoparticles by terminal and internal alkyne can equally modulate the catalytic activity towards hydrogenation of styrene by selectively covering the specific metal sites. These results demonstrate the importance of the surface and interface engineering of metal catalyst in tuning the electronic structure, surface structure and catalytic activity.

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Enhancing energy storage efficiency in lead-free dielectric ceramics through relaxor and lattice strain engineering

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Journal of Materiomics 2024年第6期10卷 1196-1205页

作者： Xuetian Gong Chao Zhang Dong Su Wenrong Xiao Fangjie Cen Ying Yang Shenglin Jiang Jing Wang kanghua Li Guangzu Zhang School of Integrated Circuits Engineering Research Center for Functional Ceramics MOE and Wuhan National Laboratory for OptoelectronicsHuazhong University of Science and TechnologyWuhanHubei430074China College of Chemnistry and Materials Science Hebei UniversityBaodingHebei071002China Key Lab of Functional Materials for Electronic Information(B) Ministry of EducationWuhanHubei430074China

Dielectric capacitors with high power density and fast charge-discharge speed play an essential role in the development of pulsed power *** increased demands for miniaturization and practicality of pulsed power equipment also necessitate the development of dielectric materials that possess high energy density while maintaining ultrahigh efficiency(η).In particular,ultrahigh efficiency signifies minimal energy loss,which is essential for practical applications but challenging to effectively ***,we demonstrate a strategy of incorporating heterovalent elements into Ba(Zr_(0.1)Ti_(0.9))O_(3),which contributes to achieving relaxor ferroelectric ceramics and reducing lattice strain,thereby improving the comprehensive energy storage ***,optimal energy storage performance is attained in 0.85Ba(Zr_(0.1)Ti_(0.9))O_(3)-0.15Bi(Zn_(2/3)Ta_(1/3))O_(3)(BZT-0.15BiZnTa),with an ultrahighηof 97.37%at 440 kV/cm(an advanced level in the lead-free ceramics)and an excellent recoverable energy storage density(Wrec)of 3.74 J/cm^(3).Notably,the BZT-0.15BiZnTa ceramics also exhibit exceptional temperature stability,maintaining fluctuations in Wrec within∼10%andηconsistently exceeding 90% across the wide temperature range of−55℃ to 160℃,and under a high electric field of 250 kV/*** these features demonstrate that the relaxor and lattice strain engineering strategies have been successful in achieving high-performance lead-free ceramics,paving the way for designing high-efficiency dielectric capacitors with a wide temperature range.

关键词： Energy storage Relaxor ferroelectrics Lead-free ceramics Lattice strain engineering

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Robust,self-adhesive,and low-contact impedance polyvinyl alcohol/polyacrylamide dual-network hydrogel semidry electrode for biopotential signal acquisition

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SmartMat 2024年第2期5卷 67-82页

作者： Guangli Li Ying Liu Yuwei Chen Yonghui Xia Xiaoman Qi Xuan Wan Yuan Jin Jun Liu Quanguo He kanghua Li Jianxin Tang Hunan Key Laboratory of Biomedical Nanomaterials and Devices College of Life Sciences and ChemistryHunan University of TechnologyZhuzhouChina Department of Neurology Zhuzhou People's HospitalZhuzhouChina Zhuzhou Institute for Food and Drug Control ZhuzhouChina

Herein,we fabricated a flexible semidry electrode with excellent mechanical performance,satisfactory self-adhesiveness,and low-contact impedance using physical/chemical crosslinked polyvinyl alcohol/polyacrylamide dual-network hydrogels(PVA/PAM DNHs)as an efficient saline *** resultant PVA/PAM DNHs showed admirable adhesive and compliance to the hairy scalp,facilitating the establishment of a robust electrode/skin interface for biopotential signal ***,the PVA/PAM DNHs steadily released trace saline onto the scalp to achieve the minimized potential drift(1.47±0.39 mV/min)and low electrode–scalp impedance(18.2±8.9 kΩ@10 Hz).More importantly,the application feasibility of real-world brain−computer interfaces(BCIs)was preliminarily validated by 10 participants using two classic BCI *** mean temporal cross-correlation coefficients between the semidry and wet electrodes in the eyes open/closed and the N200 speller paradigms are 0.919±0.054 and 0.912±0.050,*** electrodes demonstrate anticipated neuroelectrophysiological responses with similar *** semidry electrode could also effectively capture robust P-QRS-T peaks during electrocardiogram *** their outstanding advantages of fast setup,user-friendliness,and robust signals,the proposed PVA/PAM DNH-based electrode is a promising alternative to wet electrodes in biopotential signal acquisition.

关键词： brain-computer interface dual-network hydrogel electrocardiogram signals electroencephalography signals semidry electrode

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基于β-环糊精与偶氮苯衍生物的超分子囊泡体系的构筑

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化学研究 2018年第2期29卷 182-188页

作者：娄凌云苗康华杜光焰西南石油大学化学化工学院四川成都610500 西北大学化学化工学院陕西西安710069

运用铜催化的叠氮-炔基Husigen-Click环加成反应,首先设计合成了具有环糊精与三联吡啶基团的化合物A,使其同时具有了主客体识别位点和金属—离子配位位点,接着合成了具有烷基链的偶氮苯衍生物B,通过自组装,化合物A与B形成超分子聚集体.... 详细信息

运用铜催化的叠氮-炔基Husigen-Click环加成反应,首先设计合成了具有环糊精与三联吡啶基团的化合物A,使其同时具有了主客体识别位点和金属—离子配位位点,接着合成了具有烷基链的偶氮苯衍生物B,通过自组装,化合物A与B形成超分子聚集体.在A与B物质的量之比为1∶1时,其在H2O与四氢呋喃(THF)混合溶剂中可自组装形成具有双层膜结构的囊泡,并观察了囊泡在室温下的稳定性.可以通过调节紫外/可见光照控制该囊泡体系的结构,通过加入Fe2+使囊泡解组装.此外,我们通过Job's曲线证明A与B进行了1∶1包合,通过紫外滴定法表明加入Fe2+后的体系中,A与Fe2+离子的配位比为2∶1.

关键词： β-环糊精 Click反应偶氮苯自组装

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五部中国当代音乐作品中的音列思维探赜

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音乐艺术（上海音乐学院学报） 2024年第3期 4-26页

作者：刘康华中央音乐学院北京430042

“音列-特定结构模式的音的横向集合体”是作曲家个性化音高组织的基础性材料之一,“音列思维”是指作曲家在创作中恪守特定结构音列的音高组织思维方法。沈葉的唢呐协奏曲《一枝花》、姚晨的管弦乐曲《造园》、张千一的交响套曲《我的... 详细信息

“音列-特定结构模式的音的横向集合体”是作曲家个性化音高组织的基础性材料之一,“音列思维”是指作曲家在创作中恪守特定结构音列的音高组织思维方法。沈葉的唢呐协奏曲《一枝花》、姚晨的管弦乐曲《造园》、张千一的交响套曲《我的祖国》第四乐章《春到边寨》、秦文琛为管弦乐队而作的舞蹈组曲《伶伦作乐图》、郭文景的六重奏《寒山》,上述作品虽然在创作观念、精神内涵、表现内容、写作技法等方面各具特色,但在音高组织思维,即结构的深层次方面,表现出可供探讨的共性问题——音列思维。

关键词：音列音列思维传统音乐元素

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家国一体的天下秩序及其理论逻辑——以《白虎通》为中心的考察

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孔子研究 2024年第1期 39-47,157,158页

作者：左康华朱林锋广州大学马克思主义学院广州510006 吉林大学哲学社会学院长春130000

秦汉之际社会秩序的剧烈变化使传统的“家国同构”模式遭遇严重挑战,如何在帝制中国重新建构起规范齐整的伦常秩序、社会秩序以及政治秩序,成为两汉之际统治者和思想家们面临的难题。伴随着礼治原则的确立与礼治秩序的延伸,以《白虎通... 详细信息

秦汉之际社会秩序的剧烈变化使传统的“家国同构”模式遭遇严重挑战,如何在帝制中国重新建构起规范齐整的伦常秩序、社会秩序以及政治秩序,成为两汉之际统治者和思想家们面临的难题。伴随着礼治原则的确立与礼治秩序的延伸,以《白虎通》为中心,东汉思想家们建立“三纲六纪”之说,在重构伦常关系的基础上,通过更为严密的理论逻辑,使帝制时代家、国之间的嵌合变得合理而可信,兼具文化意义和政治意义的“家国一体”模式真正出现在古代中国。《白虎通》构建的家国一体的天下秩序,奠定了中国人的天下观与家国观,逐渐成为一种社会心理和文化共识,也为新时期家国观的建构提供了重要资源。

关键词：家国同构家国一体三纲六纪《白虎通》

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