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Synthesis and applications of carbon nanospheres:A review

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Particuology 2024年第4期87卷 325-338页

作者： Yaqi Yao Jinming Xu yanqiang huang Tao Zhang State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China

The synthesis of carbon nanospheres(CNS)has developed rapidly in recent years,and they are widely used owing to the tunability of their porous structures and surface properties and the unique hydrodynamic advantages conferred by their spherical *** review summarizes the methods used to synthesize CNS and their applications in various *** review first describes the four main methods of CNS synthesis,*** template,spray-drying,hydrothermal carbonization,Stöber and chemical vapor depo-sition ***,applications in the fields of energy storage,adsorption,biological medicine,and catalysis are ***,some insights on the development and design of CNS are presented.

关键词： Carbon nanosphere Synthesis Application

Effect of reduction pretreatment on the structure and catalytic performance of Ir-In_(2)O_(3)catalysts for CO_(2) hydrogenation to methanol

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Journal of Environmental Sciences 2024年第6期140卷 2-11页

作者： Changyu Ding Feifei Yang Xue Ye Chongya Yang Xiaoyan Liu Yuanlong Tan Zheng Shen Hongmin Duan Xiong Su yanqiang huang CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China

In_(2)O_(3)has been found a promising application in CO_(2)hydrogenation to methanol,which is beneficial to the utilization of CO_(2).The oxygen vacancy(O_(v))site is identified as the catalytic active center of this ***,there remains a great challenge to understand the relations between the state of oxygen species in In_(2)O_(3)and the catalytic performance for CO_(2)hydrogenation to *** the present work,we compare the properties of multiple In_(2)O_(3)and Ir-promoted In_(2)O_(3)(Ir-In_(2)O_(3))catalysts with different Ir loadings and after being pretreated under different reduction *** CO_(2)conversion rate of Ir-In_(2)O_(3)is more promoted than that of pure In_(2)O_(3).With only a small amount of Ir loading,the highly dispersed Ir species on In_(2)O_(3)increase the concentration of O_(v)sites and enhance the *** finely tuning the catalyst structure,Ir-In_(2)O_(3)with an Ir loading of 0.16 wt.%and pre-reduction treatment under 300℃exhibits the highest methanol yield of 146 mgCH_(3)OH/(gcat·hr).Characterizations of Raman,electron paramagnetic resonance,X-ray photoelectron spectroscopy,CO_(2)-temperature programmed desorption and CO_(2)-pulse adsorption for the catalysts confirm that more O_(v)sites can be generated under higher reduction temperature,which will induce a facile CO_(2)adsorption and desorption *** performance for methanol production requires an adequate dynamic balance among the surface oxygen atoms and vacancies,which guides us to find more suitable conditions for catalyst pretreatment and reaction.

关键词： Carbon dioxide Hydrogenation Methanol In_(2)O_(3) Fixed-bed Reduction temperature

Regeneration of copper catalysts mediated by molybdenum-based oxides

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Journal of Energy Chemistry 2024年第8期95卷 618-625,I0013页

作者： Changyu Ding Xiaoli Pan Isla E.Gow Xia Wu Hongchen Cao Zhounan Yu Xiaoyan Liu Xiaofeng Yang Qinggang Liu yanqiang huang CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China Cardiff Catalysis Institute School of ChemistryTranslational Research HubCardiff UniversityCardiff CF244HQUnited Kingdom College of Chemistry Chemical Engineering and Resource UtilizationNortheast Forestry UniversityHarbin 150040HeilongjiangChina

Cu catalysts,known for their unparalleled catalytic capabilities due to their unique electronic structure,have faced inherent challenges in maintaining long-term effectiveness under harsh hydrogenation ***,we demonstrate a molybdenum-mediated redispersion behavior of Cu under hightemperature oxidation *** oxidized Cu nanoparticles with rich metal-support interfaces tend to dissolve into the MoO_(3)support upon heating to 600℃,which facilitates the subsequent regeneration in a reducing atmosphere.A similar redispersion phenomenon is observed for Cu nanoparticles supported on Zn O-modified MoO_(3).The modification of ZnO significantly improves the performance of the Cu catalyst for CO_(2)hydrogenation to methanol,with the high activity being well maintained after four repeated oxidation-reduction *** situ spectroscopic and theoretical analyses suggest that the interaction involved in the formation of the copper molybdate-like compound is the driving force for the redispersion of *** method is applicable to various Mo-based oxide supports,offering a practical strategy for the regeneration of sintered Cu particles in hydrogenation applications.

关键词： Cu-based catalysts Aggregation Regeneration Oxidation CO_(2)hydrogenation

“原儒”视域下的“中国哲学史”探源——熊十力晚年思想定论

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文史哲 2024年第1期 76-91,166页

作者：黄燕强武汉大学哲学学院湖北武汉430072

“儒”和“儒学”的溯源问题,关系到如何界定中国文化思想的本源及其宗脉。熊十力《原儒》一书在探寻儒学的本源时,阐述了他对“中国文化向何处去”“中国向何处去”等时代问题的省思。围绕此中心议题而展开的,一是以“哲学”界定儒学... 详细信息

“儒”和“儒学”的溯源问题,关系到如何界定中国文化思想的本源及其宗脉。熊十力《原儒》一书在探寻儒学的本源时,阐述了他对“中国文化向何处去”“中国向何处去”等时代问题的省思。围绕此中心议题而展开的,一是以“哲学”界定儒学的知识性质,称儒学开启了中国轴心时代“哲学的突破”的序幕;二是梳理儒学在先秦的分派,藉此重建一种具备现代性的儒家学统;三是确认《易》为中国哲学之源,称《易》奠定了中国哲学的特质及其核心问题;四是论证诸子为儒家的“支与流裔”,儒学与诸子学的源流关系,呈现了先秦哲学史中经与子之间的互动互渗现象。熊十力的“原儒”既以儒学为正统,又尝试融通儒学(经学)与诸子学,从而建构一种具备现代性的新学统,由此开出科学、民主、平等等价值观念。

关键词：熊十力原儒学统《易》经子关系

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晶相设计钌基纳米催化剂提高CO2甲烷化活性（英文）

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Chinese Journal of Catalysis 2024年第06期61卷 226-236页

作者：杨冲亚王玮珏卓红英沈铮张天雨杨小峰黄延强中国科学院大连化学物理研究所中国科学院航天催化材料重点实验室中国科学院大学北京林业大学环境科学与工程学院

金属纳米颗粒在许多化学反应中表现出优异的催化性能,因而广泛用于能源和环境等催化领域.形貌是影响其催化行为的关键因素之一,它通过改变金属纳米颗粒表层原子排列结构,进而调控化学反应过程中的物质吸附、催化机理和反应动力学.此外,... 详细信息

金属纳米颗粒在许多化学反应中表现出优异的催化性能,因而广泛用于能源和环境等催化领域.形貌是影响其催化行为的关键因素之一,它通过改变金属纳米颗粒表层原子排列结构,进而调控化学反应过程中的物质吸附、催化机理和反应动力学.此外,由于金属存在多种晶相结构,其纳米颗粒暴露的表面结构也可通过改变晶相得以实现.该调控策略可使得纳米颗粒具有独特的表面结构,并展现出不同的催化性能.因此,金属纳米颗粒的晶相设计为优化金属催化剂的催化性能提供了一种有效方式.Ru基纳米催化剂对CO2甲烷化反应具有较好的活性和选择性,且密堆积的Ru（0001）晶面被证明是hcp相Ru纳米催化剂的活性中心,而（10-11）面对CO2甲烷化反应的贡献较小.因此,开发具有更丰富密堆积fcc-（111）表面的Ru基纳米催化剂,有望大幅提高CO2甲烷化的活性.本文首先通过密度泛函理论计算和微观动力学模拟,研究了fcc相Ru纳米催化剂的密堆积（111）晶面上CO2加氢反应的催化机理.结果表明,与hcp-（0001）相比,该密堆积的fcc-（111）表面因能促进CO2的吸附活化,而具有更好的CO2甲烷化反应活性.制备了具有完全暴露fcc-（111）晶面的二十面体Ru金属纳米颗粒,并将其负载于惰性载体氧化铝上,结果表明,CO2甲烷化活性比传统六方密堆积相（hcp）的钌基催化剂高5-8倍,证实了fcc相催化剂具有更高的甲烷化催化性能,同时,在较高的反应温度下,fcc-晶相的Ru基催化剂在初始反应阶段甲烷化反应活性逐渐下降,但其CO2甲烷化活性仍远高于hcp-相催化剂.原位X射线衍射和环境透射电镜等结果表明,在反应温度高于250℃条件下,fcc-晶相的金属催化剂发生部分晶相转变.该相变主要发生于Ru金属纳米颗粒的聚集体,并伴随着金属粒子的团聚和粒径的增长;然而,单颗粒分散的Ru纳米粒子在相同条件下仍能维持其fcc-晶相,从而确保了其较高的甲烷化活性.此外,原位红外结果进一步证实了CO2甲烷化在Ru基纳米催化剂上通过氢化生成HCOO*中间体的反应路径,以及Ru纳米颗粒在反应过程中的动态结构演化.综上,金属纳米颗粒的晶相设计是调控表面原子结构及其催化反应性能的有效手段.通过对Ru基纳米催化剂的晶相设计,可以显著提升其在CO2甲烷化反应中的催化活性.然而,潜在的高温晶相转变可导致催化剂活性的部分失活.总之,晶相设计通过对金属纳米粒子表面原子结构的调变,为高效催化剂的设计开发和反应机理的深入研究提供了新的机遇.

关键词：晶相设计面心立方相钌纳米催化剂二氧化碳甲烷化相变

K修饰MoS_(2)催化剂用于CO_(2)高选择性加氢制甲醇

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物理化学学报 2024年第7期40卷 58-60页

作者：杨菲菲周维杨超然张天雨黄延强中国矿业大学化工学院江苏徐州221116 北京林业大学环境科学与工程学院水体污染源控制技术北京市重点实验室北京100083 北京林业大学环境科学与工程学院污染水体源控和生态修复工程研究中心北京100083 中国科学院大连化学物理研究所应用催化重点实验室辽宁大连116023

在CO_(2)加氢领域,MoS_(2)催化剂表现出独特的潜力。然而MoS_(2)的边缘S空位对CH_(4)的生成更有利,这限制了目标产物甲醇的选择性。本工作中,我们发现,通过掺杂K助剂可以显著提高MoS_(2)催化CO_(2)选择性加氢制甲醇的性能,而未修饰的MoS... 详细信息

在CO_(2)加氢领域,MoS_(2)催化剂表现出独特的潜力。然而MoS_(2)的边缘S空位对CH_(4)的生成更有利,这限制了目标产物甲醇的选择性。本工作中,我们发现,通过掺杂K助剂可以显著提高MoS_(2)催化CO_(2)选择性加氢制甲醇的性能,而未修饰的MoS_(2)主要产生CH_(4)。通过一系列的表征研究,我们发现,K原子更倾向于稳定在MoS_(2)的边缘位点上,并向MoS_(2)转移电子,从而增强了MoS_(2)边缘位点的碱性。这有助于CO_(2)的吸附活化,并以较低的能垒解离为CO。此外,K助剂还有助于调控CO中间体定向转化为甲醇而非CH_(4)。这一发现拓展了MoS_(2)材料在CO_(2)合成甲醇中的应用。通过掺杂K助剂,我们能够更高效地利用MoS_(2)催化CO_(2)转化为甲醇,对于减缓气候变化和开发清洁能源具有重要意义。

关键词： CO_(2)加氢甲醇甲烷选择性调控 K-MoS_(2)

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Structural reconstruction of Sn-based metal-organic frameworks for efficient electrochemical CO_(2) reduction to formate

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Chinese Journal of Chemical Engineering 2022年第3期35卷 353-359页

作者： Yachen Deng Shifu Wang yanqiang huang Xuning Li State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

MOF-based materials have been widely explored in electrochemical CO_(2)reduction reactions for the production of valuable *** the reconstruction of those catalysts under working conditions is crucial for the identification of active sites and clarification of reaction ***,a series of six N coordinated Sn-based metal-organic frameworks(Sn-N6-MOFs)are newly developed for electrochemical CO_(2)reduction(CO_(2)RR).2%Sn-N6-MOF achieves the optimal catalytic performance with a formate Faradaic efficiency of~85%and a current density of 23 mA·cm^(-2) at-1.23 V ***-situ Raman results combined with ex-situ ^(119)Sn Mössbauer measurements reveal the structural reconstruction of Sn-N6-MOFs during CO_(2)RR,generating tin nanoclusters as the real active sites for CO_(2)electroreduction to HCOOH.

关键词： Structural reconstruction Metal-organic frameworks Mössbauer spectroscopy Electrochemical CO_(2)reduction

植物源黄酮类化合物对幽门螺杆菌脲酶抑制作用的研究进展

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医药导报 2024年第8期43卷 1309-1314页

作者：徐文艳黄干荣廖丽娟罗家锱黄亮黄衍强右江民族医学院广西病原微生物耐药防控科技创新合作基地广西高校耐药微生物感染防治研究重点实验室百色533000

脲酶作为氮循环的关键酶,为生物体提供生长所需的氮源,同时也是一种在各种致病菌中发现的毒力因子。幽门螺杆菌(***)产生的脲酶为其在胃里的定植和生存中起着重要作用,而幽门螺杆菌的感染与肠化生、活动性胃炎、消化性溃疡和胃癌等胃肠... 详细信息

脲酶作为氮循环的关键酶,为生物体提供生长所需的氮源,同时也是一种在各种致病菌中发现的毒力因子。幽门螺杆菌(***)产生的脲酶为其在胃里的定植和生存中起着重要作用,而幽门螺杆菌的感染与肠化生、活动性胃炎、消化性溃疡和胃癌等胃肠道疾病密切相关,且随着耐药性菌株的增多,迫切需要治疗有效、安全的新型药物,所以幽门螺杆菌成为最常研究的产脲酶细菌之一,脲酶作为抗菌药物的潜在靶点也受到关注。安全性较高的药用植物已被证明具有治疗潜力,许多植物天然提取物已成为新型药物开发的灵感和起点,以往研究还发现许多天然存在的黄酮类化合物具有抗脲酶活性。该文概述了一些植物源黄酮类化合物对幽门螺杆菌脲酶的抑制作用,根据其来源、结构特点以及可能的作用机制,寻找和开发植物来源且特异性抗幽门螺杆菌的化合物,从而为临床候选药物的研发提供参考。

关键词：黄酮类化合物幽门螺杆菌脲酶抗菌作用

Preface to special column on catalytic conversion of CO_(2)

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Chinese Journal of Catalysis 2022年第7期43卷 1545-1546页

作者： yanqiang huang Da-Gang Yu Guoxiong Wang CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Key Laboratory of Green Chemistry&Technology of Ministry of Education College of ChemistrySichuan University State Key Laboratory of Catalysis CAS Center for Excellence in NanoscienceDalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of Sciences

With the increasing awareness of sustainable chemistry and green chemistry,catalytic conversion of carbon dioxide(CO_(2))into high value‐added and bulk chemicals is a promising tech‐nology that can utilize CO_(2) as an ideal C1 source while simulta‐neously storing renewable *** being frustrated with its thermodynamic stability and kinetic inertness,CO_(2) has been tamed for triggering catalytic constructions of highly‐valued entities like important hydrocarbon fuels and fine chemicals,mainly aiding by two scenarios:CO_(2) reduction and CO_(2)‐involved organic ***,science,industry and govern‐ment agencies have been devoted to leverage these synthetic tools in targeting the catalytic conversion of CO_(2).Therefore,it motivates us to organize the special column of“Catalytic Con‐version of CO_(2)”.The column contains 14 papers,including 4 reviews,4 communications and 6 articles,which cover the frontiers and most of the research aspects of catalytic con‐version of CO_(2).

关键词： catalytic utilize valued