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NiO@Ni nanoparticles embedded in N-doped carbon for efficient photothermal CO_(2) methanation coupled with H_(2)O splitting

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Nano Research 2024年第4期17卷 2283-2290页

作者： Yun Zhou Peng Zheng Fang Wang fangna gu Wenqing Xu Qinyang Lu Tingyu Zhu Ziyi Zhong guangwen Xu Fabing Su Institute of Process Engineering Chinese Academy of SciencesBeijing 100190China Key Laboratory on Resources Chemicals and Materials of Ministry of Education Shenyang University of Chemical TechnologyShenyang 110142China Institute of Industrial Chemistry and Energy Technology Shenyang University of Chemical TechnologyShenyang 110142China School of Ecology and Environment Beijing Technology and Business UniversityBeijing 100048China Beijing Key Laboratory of Enze Biomass Fine Chemicals College of New Materials and Chemical EngineeringBeijing Institute of Petrochemical TechnologyBeijing 102617China International School of Beijing 10 An Hua Street Shunyi DistrictBeijing 100048China Department of Chemical Engineering Guangdong Technion Israel Institute of Technology(GTIIT)Shantou 515063China Technion Israel Institute of Technology(IIT) Haifa32000Israel

Photothermal carbon dioxide(CO_(2))methanation has attracted increasing interest in solar fuel synthesis,which employs the advantages of photocatalytic H_(2)O splitting as a hydrogen source and photothermal catalytic CO_(2) *** work prepared three-dimensional(3D)honeycomb N-doped carbon(NC)loaded with core–shell NiO@Ni nanoparticles generated in situ at 500℃(NiO@Ni/NC-500).Under the photothermal catalysis(200℃,1.5 W/cm^(2)),the CH_(4) evolution rate of NiO@Ni/NC-500 reached 5.5 mmol/(g·h),which is much higher than that of the photocatalysis(0.8 mmol/(g·h))and the thermal catalysis(3.7 mmol/(g·h)).It is found that the generated localized surface plasmon resonance enhances the injection of hot electrons from Ni to NiO,while thermal heating accelerates the thermal motion of radicals,thus generating a strong photo-thermal synergistic effect on the *** CO_(2) reduction to CH_(4) follows the*OCH *** work demonstrates the synergistic effect of NiO@Ni and NC can enhance the catalytic performance of photothermal CO_(2) reduction reaction coupled with water splitting reaction.

关键词： Ni localized surface plasmon resonance photothermal methanation

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Ordered mesoporous Cu-Ca-Zr:A superior catalyst for direct synthesis of methyl formate from syngas

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Carbon Resources Conversion 2018年第2期1卷 174-182页

作者： Jiahao Zhuang Bin Lu fangna gu Ziyi Zhong Fabing Su State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China Zhongke Langfang Institute of Process Engineering Fenghua Road No.1Langfang Economic&Technical Development ZoneHebei Province 065001China Institute of Chemical and Engineering Sciences Agency for ScienceTechnology and Research(A*STAR)1 Pesek RoadJurong IslandSingapore 627833Singapore Institute of Industrial Chemistry and Energy Technology Shenyang University of Chemical TechnologyShenyang 110142China

It is still a big challenge to obtain both highly active and stable Cu-based catalysts for direct synthesis of methyl formate(MF)from *** address the issue,we have designed and synthesized a series of ternary Cu-Ca-Zr catalysts,namely,the ordered mesoporous Cu-Ca-Zr catalyst prepared by one-pot evaporation-induced self-assembly(EISA)method,and the supported CuO/CaO-ZrO_(2)catalysts by impregnating with copper precursor or by immobilizing copper *** the latter two catalysts,the ordered mesoporous CaO-ZrO_(2)support was also prepared by the EISA *** catalysts were characterized by techniques such as ICP,XRD,TEM,N2 isotherm adsorption-desorption,XPS and H2-TPR,and used for direct synthesis of *** results indicated that the catalyst prepared by onepot EISA method,in which the CuO species are highly dispersed in frame of CaO-ZrO_(2),exhibits much better activity and stability as compared with the other two catalysts with most of CuO located on the outer surface of the CaO-ZrO_(2)support,because the former has a higher specific surface area,enhanced synergistic effect and stronger interaction between the CaO-ZrO_(2)support and CuO active constituent.

关键词： Methyl formate Direct synthesis Cu-based catalyst Ordered mesoporous Activity

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Ni/Al_2O_3 catalysts for CO methanation: Effect of Al_2O_3 supports calcined at different temperatures

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Journal of Energy Chemistry 2013年第6期22卷 919-927页

作者： Jiajian Gao Chunmiao Jia Jing Li Meiju Zhang fangna gu guangwen Xu Ziyi Zhong Fabing Su State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences University of Chinese Academy of Sciences Institute of Chemical Engineering and Sciences A*star

The correlation between phase structures and surface acidity of Al2O3 supports calcined at different temperatures and the catalytic performance of Ni/Al2O3 catalysts in the production of synthetic natural gas(SNG) via CO methanation was systematically investigated. A series of 10 wt% NiO/Al2O3 catalysts were prepared by the conventional impregnation method, and the phase structures and surface acidity of Al2O3 supports were adjusted by calcining the commercial γ-Al2O3 at different temperatures(600–1200 C). CO methanation reaction was carried out in the temperature range of 300–600 C at different weight hourly space velocities(WHSV = 30000 and 120000 mL·g-1h-1) and pressures(0.1 and 3.0 MPa). It was found that high calcination temperature not only led to the growth in Ni particle size, but also weakened the interaction between Ni nanoparticles and Al2O3 supports due to the rapid decrease of the specific surface area and acidity of Al2O3 supports. Interestingly, Ni catalysts supported on Al2O3 calcined at 1200 C(Ni/Al2O3-1200) exhibited the best catalytic activity for CO methanation under different reaction conditions. Lifetime reaction tests also indicated that Ni/Al2O3-1200 was the most active and stable catalyst compared with the other three catalysts, whose supports were calcined at lower temperatures(600, 800 and 1000 C). These findings would therefore be helpful to develop Ni/Al2O3 methanation catalyst for SNG production.

关键词： Ni catalyst alumina CO methanation synthetic natural gas carbon deposition

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In-situ growth of heterophase Ni nanocrystals on graphene for enhanced catalytic reduction of 4-nitrophenol

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Nano Research 2022年第2期15卷 1230-1237页

作者： Jiahao Zhuang Feng He Xianglin Liu Pengchao Si fangna gu Jing Xu Yu Wang guangwen Xu Ziyi Zhong Fabing Su School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100049China State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Key Laboratory on Resources Chemicals and Materials of Ministry of Education Shenyang University of Chemical TechnologyShenyang 110142China State Key Laboratory of Chemical Engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China Department of Chemical Engineering Guangdong Technion-Israel Institute of Technology(GTIIT)Shantou 515063China Technion-Israel Institute of Technology(IIT) Haifa 32000Israel

Generating heterophase structures in nanomaterials,e.g.,heterophase metal nanocrystals,is an effective way to tune their physicochemical properties because of their high-energy nature and unique electronic environment of the generated ***,the direct synthesis of heterophase metal nanocrystals remains a great challenge due to their unstable ***,we report the in situar direct synthesis of heterophase Ni nanocrystals on *** heterostructure of face-centered cubic(fee)and hexagonal close-packed(hep)phase was generated via the epitaxial growth of hep Ni and the partial transformation of fee Ni and stabilized by the anchoring effect of graphene toward fee Ni nanocrystal and the preferential adsorption of surfactant polyethylenimine(PEI)toward epitaxial hep *** with the fee Ni nanocrystals grown on graphene,the heterophase(fcc/hcp)Ni nanocrystals in situ grown on graphene showed a greatly improved catalytic activity and reusability in 4-nitrophenol(4-NP)reduction to 4-aminophenol(4-AP).The measured apparent rate constant and the activity parameter were 2.958 min^(-1) and 102 min^(-1)·mg^(-1),respectively,higher than that of the best reported non-noble metal catalysts and most noble metal *** control experiments and density functional theory calculations reveal that the interface of the fee and hep phases enhances the adsorption of substrate 4-NP and thus facilitates the reaction *** work proves the novel idea for the rational design of heterophase metal nanocrystals by employing the synergistic effect of surfactant and support,and also the potential of creating the heterostructure for enhancing their catalytic reactivity.

关键词： heterophase structure Ni nanocrystals graphene 4-nitrophenol(4-NP)reduction catalysts

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Coking-resistant Ni-ZrO_2/Al_2O_3 catalyst for CO methanation

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Journal of Energy Chemistry 2014年第6期23卷 761-770页

作者： Qing Liu fangna gu Jiajian Gao Huifang Li guangwen Xu Fabing Su State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences

Highly coke-resisting ZrO2-decorated Ni/A1203 catalysts for CO methanation were prepared by a two-step process. The support was first loaded with NiO by impregnating method and then modified with ZrO2 by deposition-precipitation method （IM-DP）. Nitrogen adsorption- desorption, X-ray diffraction, scanning electron microscopy, transmission electron microscopy, thermogravimetdc analysis, H2 temperature- programmed reduction and desorption, NH3 temperature-programmed desorption, and zeta potential analysis were employed to characterize the samples. The results revealed that, compared with the catalysts with the same composition prepared by co-impregnation （CI） and sequential impregnation （SI） methods, the Ni/A1203 catalyst prepared by IM-DP showed much enhanced catalytic performance for syngas methanation under the condition of atmospheric pressure and a high weight hourly space velocity of 120000 mL.g-1 .h-1. In a 80 h life time test under the condition of 300-600 ~C and 3.0 MPa, this catalyst showed high stability and resistance to coking, and the amount of deposited carbon was only 0.4 wt%. On the contrary, the deposited carbon over the catalyst without ZrO2 reached 1.5 wt% after a 60 h life time test. The improved catalytic performance was attributed to the selective deposition of ZrO2 nanoparticles on the surface of NiO rather than A1203, which could he well controlled via changing the electrostatic interaction in the DP procedure. This unique structure could enhance the dissociation of CO2 and generate surface oxygen intermediates, thus preventing carbon deposition on the Ni particles in syngas methanation.

关键词： Ni/γ-A1203 ZrO2 coke resistance syngas methanation

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ZrO_2-modified Ni/LaAl_(11)O_(18) catalyst for CO methanation: Effects of catalyst structure on catalytic performance

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Chinese Journal of Catalysis 2018年第2期39卷 297-308页

作者： Hongmei Ai Hongyuan Yang Qing Liu guoming Zhao Jing Yang fangna gu Key Laboratory of Low Carbon Energy and Chemical Engineering College of Chemical and Environmental Engineering Shandong University of Science and Technology Qingdao 266590 Shandong China Assets Management Division Shandong University of Science and Technology Qingdao 266590 Shandong China State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 China

We report Ni/LaHA@ZrO2catalysts prepared by a facile modified successive adsorption and reaction method for CO methanation.N2adsorption,X‐ray diffraction,transmission electron microscopy,scanning electron microscopy,thermogravimetric analysis,H2temperature‐programmed reduction,H2temperature‐programmed desorption,X‐ray photoelectron spectroscopy,thermogravimetric analysis,and inductively coupled plasma atomic emission spectrometry were used to characterize the *** results indicated that the ZrO2nanoparticles were distributed over the surface of the Ni/LaHA@ZrO2catalyst and even partially covered some Ni particles,resulting in the coating exerting a confinement *** excess ZrO2had an adverse effect on the enhancement of CO conversion because of the coverage of the surface Ni particles;however,the Ni/LaHA@ZrO2catalyst displayed much higher CH4selectivity than Ni/LaHA because of the activation of the byproduct CO2molecules by ***,even though20Ni/LaHA@ZrO2‐5exhibited similar CO conversion as20Ni/LaHA,the use of the former resulted in a higher CH4yield than the use of the latter.A107‐h‐lifetime test revealed that the Ni/LaHA@ZrO2catalyst was highly stable with superior anti‐sintering and anti‐coking properties because of its coating structure and the promoter effect of ZrO2.

关键词： Lanthanum hexaaluminate ZrO2 Nickel catalyst Coating structure CO methanation

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调控介孔硅分子筛的孔壁结构以提高吸附亚硝胺的效率

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催化学报 2010年第3期31卷 267-272页

作者：古芳娜杨佳园魏峰朱建华南京大学化学化工学院介观化学教育部重点实验室江苏南京210093

针对高空速下捕获痕量毒物分子的环境净化要求,尝试调控介孔材料孔壁结构以提高其吸附小分子环境污染物的效率.通过调节合成体系的pH值、加入无机盐以及控制表面活性剂浓度等方法,改变硅物种与模板剂胶束的组装速度或无机-有机液晶相的... 详细信息

针对高空速下捕获痕量毒物分子的环境净化要求,尝试调控介孔材料孔壁结构以提高其吸附小分子环境污染物的效率.通过调节合成体系的pH值、加入无机盐以及控制表面活性剂浓度等方法,改变硅物种与模板剂胶束的组装速度或无机-有机液晶相的存在形态,研制含有孔壁缺陷位的介孔分子筛新材料.通过X射线衍射和低温氮气吸附研究了样品的结构特性,并采用高分辨透射电镜和固体核磁技术证实了介孔材料孔壁缺陷位的形成.以挥发性吡咯烷亚硝胺为靶标分子,考察了所得材料的吸附性能.结果表明,大量缺陷空位的存在成倍地提高了介孔分子筛吸附挥发性亚硝胺的效率,为设计研制环保新材料提供了新思路.

关键词： MCM-41介孔分子筛孔壁结构缺陷位亚硝胺吸附

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一锅法制备高活性高稳定性Ni-Nd-Al三元有序介孔甲烷化催化剂

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化工学报 2017年第10期68卷 3823-3831页

作者：庄嘉豪靳国静古芳娜贾丽华苏发兵中国科学院过程工程研究所多相复杂系统国家重点实验室北京100190 中国科学院大学北京100049 齐齐哈尔大学化学与化学工程学院黑龙江齐齐哈尔161006

CO甲烷化在煤制天然气技术中起着重要作用,Ni基催化剂作为目前研究最多的甲烷化催化剂,仍存在低温活性差、高温易烧结和易积炭等问题。针对这些问题,采用改进的溶剂蒸发诱导自组装方法,设计制备了不同含量Nd物种修饰的Ni-Nd-Al三元有序... 详细信息

CO甲烷化在煤制天然气技术中起着重要作用,Ni基催化剂作为目前研究最多的甲烷化催化剂,仍存在低温活性差、高温易烧结和易积炭等问题。针对这些问题,采用改进的溶剂蒸发诱导自组装方法,设计制备了不同含量Nd物种修饰的Ni-Nd-Al三元有序介孔甲烷化催化剂。采用N_2-物理吸附、X射线衍射(XRD)、X射线光电子能谱(XPS)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)等分析方法对反应前后催化剂的结构和形貌进行了表征,并考察其CO甲烷化反应催化性能。结果表明,制备出的Ni-Nd-Al甲烷化催化剂均具有有序介孔结构,Ni和Nd物种均匀分布在孔道内。适量Nd物种的加入有助于减小Ni颗粒的尺寸,提高其分散度和对H_2的吸附能力,进而提升催化剂的活性。有序介孔结构的限域效应有助于提高催化剂抗烧结和抗积炭能力。

关键词： Ni基催化剂介孔结构制备 CO甲烷化活性稳定性

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CO_(2)甲烷化镍基催化剂研究进展

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洁净煤技术 2022年第4期28卷 1-17页

作者：张晓俐古芳娜苏发兵许光文沈阳化工大学资源化工与材料教育部重点实验室辽宁沈阳110142 中国科学院过程工程研究所多相复杂系统国家重点实验室北京100190 沈阳化工大学能源与化工产业技术研究院辽宁沈阳110142

CO_(2)甲烷化技术不仅可以实现CO_(2)的循环利用,还能解决CO_(2)排放带来的环境问题。近年来,Ni基催化剂因催化活性好、甲烷选择性高和价格低廉等优点被广泛应用于CO_(2)甲烷化反应中。重点阐述了Ni颗粒的尺寸效应、表面微细结构、载体... 详细信息

CO_(2)甲烷化技术不仅可以实现CO_(2)的循环利用,还能解决CO_(2)排放带来的环境问题。近年来,Ni基催化剂因催化活性好、甲烷选择性高和价格低廉等优点被广泛应用于CO_(2)甲烷化反应中。重点阐述了Ni颗粒的尺寸效应、表面微细结构、载体种类及物理化学性质(碱性位、氧空位、比表面积、孔结构和金属-载体间相互作用)对CO_(2)甲烷化催化剂催化性能的影响,介绍了Ni基双金属合金、结构和电子型助剂对其催化性能的影响,归纳了不同催化剂上CO_(2)甲烷化机理,剖析了Ni基催化剂失活的原因,论述了Ni基催化剂在光热催化CO_(2)甲烷化中的应用,最后对CO_(2)甲烷化催化剂未来研究方向进行了展望。通过对比不同体系获得的研究结果发现,CO_(2)甲烷化反应为结构敏感性反应,Ni颗粒尺寸对催化剂活性有显著影响,然而不同研究得出的最佳Ni颗粒尺寸有明显差异,这可能与不同金属与载体间相互作用或不同制备方法导致的Ni颗粒表面微细结构(如不同晶面、缺陷位等)差异有关,Ni颗粒的尺寸效应有待深入研究;第二金属的加入形成Ni基双金属合金、助剂及研究金属-载体相互作用都有助于开发高稳定性的催化剂;载体表面丰富的碱性位及氧空位,有利于CO_(2)吸附与活化,进而提高催化剂活性。目前,CO_(2)甲烷化反应路径主要分为CO路径和甲酸盐路径,反应遵循的路径可能与反应条件(如温度、压力等)及催化剂表面性质(如羟基丰富度、O^(2-)吸附位点等)有关。然而,关于助剂或载体与Ni物种间的纳米界面结构,以及采用不同助剂和载体对催化剂活性位点及CO_(2)甲烷化反应路径的影响机制,尚缺乏较深入的认知。因此,需借助现场原位成像技术及光谱学技术对催化剂的表界面几何与电子结构进行精细、动态的结构剖析,建立动态结构与性能的构效关系,有利于指导设计合成特定结构的高效Ni基催化剂。

关键词： CO_(2)甲烷化镍基催化剂光热催化第二金属载体催化活性

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二氧化碳甲烷化催化剂及反应机理研究进展

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过程工程学报 2023年第3期23卷 375-395页

作者：田郡博古芳娜苏发兵张战国许光文沈阳化工大学资源化工与材料教育部重点实验室辽宁沈阳110142 中国科学院过程工程研究所多相复杂系统国家重点实验室北京100190 沈阳化工大学能源与化工产业技术研究院辽宁沈阳110142

在“双碳”目标的背景下,明确碳处理路径至关重要。利用可再生能源制得的氢,将二氧化碳(CO_(2))通过甲烷化反应制备合成天然气(SNG)被广泛认为是一种高效、有前景的碳捕集利用技术,有望实现碳循环利用。近年来,二氧化碳甲烷化催化剂及... 详细信息

在“双碳”目标的背景下,明确碳处理路径至关重要。利用可再生能源制得的氢,将二氧化碳(CO_(2))通过甲烷化反应制备合成天然气(SNG)被广泛认为是一种高效、有前景的碳捕集利用技术,有望实现碳循环利用。近年来,二氧化碳甲烷化催化剂及相关反应机理均取得了许多新进展。鉴于此,本工作对该反应进行了系统的综述。首先,介绍了CO_(2)甲烷化反应的热力学研究中不同反应条件的影响;随后从活性金属、载体、制备方法及辅助技术等四方面介绍了CO_(2)甲烷化催化剂的研究进展,其中活性组分包括非贵金属基(Ni,Fe,Co和Mo)和贵金属基(Ru,Rh,Pt和Pd),载体包括传统氧化物(Al2O3,SiO_(2),TiO_(2),ZrO_(2)和CeO_(2))和新型载体材料(金属有机框架和碳基材料),催化剂制备方法包括传统制备方法(浸渍法、共沉淀法、水热法、溶胶-凝胶法和固相合成法)和合成辅助技术(超声波、微波和等离子体等);总结了CO_(2)甲烷化反应遵循的两条机理路径(甲酸盐路径和CO路径),并指出CO_(2)甲烷化的具体反应途径与催化剂表面特性(如羟基丰富度和O_(2)-位点)和反应条件(如反应温度和压力)相关;最后提出了当前研究存在的挑战,并对研究前景作出展望。

关键词： CO_(2)甲烷化热力学催化剂制备方法反应机理

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