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Journal of Rare Earths 2021年第4期39卷 364-373页

作者： Lulu Zhou Shuai Wei Weiwei Wang Zhao Jin chunjiang jia Key Laboratory for Colloid and Interface Chemistry Key Laboratory of Special Aggregated MaterialsSchool of Chemistry and Chemical EngineeringShandong UniversityJinan 250100China

So far,it is still a controversial issue which status of gold species is a better active site for catalyzing CO ***,the influence of the different atmospheres pretreatment(oxidative and reductive)on gold state of Au/La-CeOx(1 wt%gold loading)catalyst during CO oxidation was *** changes of Au species were monitored by combined in situ diffuse reflectance infrared Fourier transform spectroscopy(in situ DRIFTS)and X-ray photoelectron spectroscopy(XPS).For the sample pretreated with oxidative atmosphere,the data show that the initial Au^(3+)is transformed to Au^(δ+)(0<δ<1)during CO oxidation,which is a key step to lead to higher *** the sample after reductive atmosphere pretreatment,Au^(δ+)is mixed with a small amount of Au^(0)which can be converted to Au^(δ+)with the increase of temperature in ***,the sample always maintains high activity during the ***,the Au®+obtained by reductive pretreatment is more active than the Au^(3+)obtained by oxidative treatment in catalyzing CO oxidation.

关键词： Au/La-CeO_(x)catalyst Pretreatment atmospheres CO oxidation Au^(δ+) Au^(3+) Rare earths

CeO_(2-x) modified Ru/γ-Al_(2)O_(3) catalysts for ammonia decomposition reaction

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Journal of Rare Earths 2023年第6期41卷 801-809,I0001页

作者： Qinglu Meng Haoxin Liu Kai Xu Weiwei Wang chunjiang jia Key Laboratory for Colloid and Interface Chemistry Key Laboratory of Special Aggregated MaterialsSchool of Chemistry and Chemical EngineeringShandong UniversityJinan 250100China

Developing high-performance ammonia decomposition catalysts for preparing COx-free hydrogen shows great practical ***,CeO_(2) is used as a promoter to modulate the metal-support interaction to enhance the catalytic performance of Ru/Al_(2)O_(3) catalysts.A series of 1Ru/xCe-10AI(x=0.5,1,or 3)catalysts was prepared by a facile colloidal deposition *** find that the optimized 1 Ru/1Ce-10Al catalyst exhibits excellent activity for the decomposition of ammonia with a very high hydrogen yield of7097 mmolH2/(gRu·min)at 450℃.It is confirmed that Ru species are highly dispersed on the support surface as stable small clusters(~1.3 nm).More importantly,due to the interaction between Ru species and partially reduced CeO_(2-x),the electron density of Ru species is increased,which is beneficial to the high activity of the 1 Ru/xCe-10Al *** work paves a way to construct high-efficiency ammonia decomposition catalysts modified by CeO_(2).

关键词： Ammonia decomposition Ru clusters CeO_(2-x)promoter Metal-support interaction Rare earths

Copper-ceria sheets catalysts: Effect of copper species on catalytic activity in CO oxidation reaction

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Journal of Rare Earths 2017年第12期35卷 1186-1196页

作者： Linying Du Weiwei Wang Han Yan Xu Wang Zhao Jin Qisheng Song Rui Si chunjiang jia Key Laboratory for Colloid and Interface Chemistry Key Laboratory of Special Aggregated Materials School of Chemistry and Chemical EngineeringShandong University Shanghai Synchrotron Radiation Facility Shanghai Institute of Applied Physics Chinese Academy of Sciences

Copper-ceria sheets catalysts with different loadings of copper（2 wt.%, 5 wt.% and 10 wt.%） supported on ceria nanosheets were synthesized via a depositioneprecipitation（DP） method. The prepared catalysts were systematically characterized with various structural and textural detections including X-ray diffraction（XRD）, Raman spectra, transmission electron microscopy（TEM）, X-ray absorption fine structure（XAFS）, and temperature-programmed reduction by hydrogen（H2-TPR）, and tested for the CO oxidation reaction. Notably, the sample containing 5 wt.% of Cu exhibited the best catalytic performance as a result of the highest number of active CuO species on the catalyst surface. Further increase of copper content strongly affects the dispersion of copper and thus leads to the formation of less active bulk CuO phase, which was verified by XRD and H2-TPR analysis. Moreover, on the basis of in-situ diffuse reflectance infrared Fourier transform spectroscopy（in-situ DRIFTS） results, the surface Cu~＋ species, which are derived from the reduction of Cu^（2＋）, are likely to play a crucial role in the catalyzing CO ***, the superior catalytic performance of the copper-ceria sheets is mainly attributed to the highly dispersed CuOx cluster rather than Cu-[Ox]-Ce structure, while the bulk CuO phase is adverse to the catalytic activity of CO oxidation.

关键词： Ceria nanosheets Copper-ceria catalysts CO oxidation Copper oxide species Structure-properties relationship

Fe- and Co-doped lanthanum oxides catalysts for ammonia decomposition:Structure and catalytic performances

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Journal of Rare Earths 2017年第1期35卷 15-23页

作者： XUN Yanran HE Xinxin YAN Han GAO Ziwang JIN Zhao jia chunjiang Key Laboratory for Colloid and Interface Chemistry Key Laboratory of Special Aggregated Materials School of Chemistry and Chemical Engineering Shan- dong University Jinan 250100 China

In this paper, a series of Fe- and Co-doped lanthanum（hydr）oxides catalysts were prepared by a simple coprecipitationhydrothermal method. The as-prepared catalysts were characterized with various techniques including powder X-ray diffraction（XRD）, N2 adsorption/desorption, inductively coupled plasma（ICP） and transmission electron microscopy（TEM）. The Fe-based catalysts exhibited consecutive phase changes of amorphous Fe Ox→FeLaO3→Fe2N under different stages（as-prepared→calcination→ammonia decomposition reaction）; as for Co-based catalysts, the phase transformation followed a sequence of Co（OH）2→Co3O4→metallic Co. It was revealed that Fe2N and metallic Co were most probably the active crystalline phase respectively for Feand Co-based catalysts in the decomposition of ammonia.

关键词： transitional metal rare earth lanthanum(hydr)oxides composite catalysts ammonia decomposition

Effect of reduction-oxidation treatment on structure and catalytic properties of ordered mesoporous Cu-Mg-Al composite oxides

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Science Bulletin 2015年第12期60卷 1108-1113,I0003页

作者： Jingting Lu Yan Zhang Chengli jiao Suresh Kumar Megarajan Dong Gu Guocheng Yang Heqing jiang chunjiang jia Ferdi Schiith School of Chemistry and Life Science Changchun University of Technology Changchun 130012 China Key Laboratory of Biobased Materials Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy ofSciences Qingdao 266101 China Max-Planck-lnstitut for Kohlenforschung Kaiser-Wilhelm-Platz 145470 Mtilheim an der Ruhr Germany Key Laboratory for Colloid and Interface Chemistry Key Laboratory of Special Aggregated Materials School of Chemistry and Chemical Engineering Shandong UniversityJinan 250100 China

Ordered mesoporous Cu-Mg-A1 composite oxides were synthesized via the one-pot evaporation-in- duced self-assembly strategy. Using this method, copper was first homogeneously incorporated into the ordered mesoporous spinel matrix. After H2 reduction treatment, according to X-ray diffraction （XRD） and transmission electron microscopy （TEM） results, copper existed as metallic nanoparticles with the size of 6-10 nm that well decorated the parent mesoporous skeleton. The metallic nanoparticles were then re-oxidized to copper oxide when exposed to air or during CO oxidation reaction at low temperatures. Thus, copper migrated from bulk spinel phase to the surface after the reduction-oxidation treat- ment. Moreover, the copper on the surface was re-incor- porated into the bulk spinel phase by further thermal treatment at much higher temperature in the presence of air. The correlation between the state of copper in the mesoporous composite oxides and the catalytic perfor- mance toward CO oxidation was studied. It was found that copper existed as oxide nanoparticles on the surface of mesoporous Mg-Al skeleton is much more active than that existed as lattice Cu ions in spinel phase.

关键词： Cu-Mg-Al oxides Evaporation-induced self-assembly Mesoporous materials Migration CO oxidation

CO oxidation over Au/ZrLa-doped CeO_2 catalysts: Synergistic effect of zirconium and lanthanum

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Chinese Journal of Catalysis 2016年第8期37卷 1331-1339页

作者：杨琦杜林颖王旭贾春江司锐中国科学院上海应用物理研究所上海光源上海210204 山东大学胶体与界面化学教育部重点实验室特种功能聚集体材料教育部重点实验室化学与化工学院山东济南250100

The physicochemical properties of nanosized Au catalysts supported on doped CeO2 and their cata‐lytic performance for the CO oxidation reaction were investigated. The Au/Zr‐doped CeO2 catalyst is much more active than undoped Au/CeO2, while Au/ZrLa‐doped CeO2 shows the highest activity. Characterization of the catalysts by X‐ray diffraction, transmission electron microscopy （TEM）, high‐resolution TEM, and the X‐ray absorption fine structure technique shows high homogeneity of the oxide supports and well‐dispersed nanosized Au nanoparticles. Raman spectroscopy, X‐ray photoelectron spectroscopy, and H2‐tempeature‐programmed reduction show that the surface oxygen species are the main factor for the catalytic activity in the CO oxidation reaction, while the supported Au species can improve the redox properties and create oxygen vacancy sites on the support. The oxidation state of Au is not the main factor governing the activity of Au/doped‐CeO2 catalysts. Additionally, the synergistic effect of Zr and La is discussed.

关键词： Gold catalyst Doped ceria Oxygen vacancy Carbon monoxide oxidation Metal-support interaction

Ensemble of single-atom catalysis and defect engineering in Cu/CeOnanozymes for tumor therapy

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Science China Chemistry 2023年

作者： Haoxin Liu Zhiliang Gao Han Yan Shanqing Li Weiwei Wang Xuetao Qin Hongning Sun Jiwei Cui chunjiang jia Key Laboratory of Colloid and Interface Chemistry Key Laboratory of Special Aggregated Materials of the Ministry of Education School of Chemistry and Chemical Engineering Shandong University School of Materials and Environmental Engineering Chizhou University

As a class of nanomaterials with natural enzyme-like characteristics, nanozymes have shown their great potential in various applications. Reducible metal oxides featured with defect structures, and single-atom catalysts with isolated metal sites are regarded as two of the most promising nanozymes. However, the strategies to construct highly performed nanozymes by combining these advantages are rarely reported. Herein, we report the coordination-unsaturated single-atomic Cu species supported on sintered CeO2, which combines the advantages of defect engineering and single-atom catalysis, exhibiting a largely enhanced peroxidase(POD)-like activity. The high-temperature calcination induces the transformation of inert Cu1O4species into coordination-unsaturated Cu1O3sites. This novel Cu1O3active sites with an unsaturated coordination work as a new type of defect sites to greatly activate the isolated Cu atoms and accelerate the dissociation of H2O2to form hydroxyl radicals(·OH). The obtained nanozyme with a high POD-like activity possesses low cytotoxicity, showing potential applications for the tumor inhibition in vitro and in vivo.

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针对氨分解反应的稀土基催化剂研究进展

中国稀土学报 2023年第3期41卷 404-415,I0001页

作者：徐凯周璐璐王伟伟贾春江胶体与界面化学教育部重点实验室特种功能聚集体材料教育部重点实验室山东大学化学与化工学院山东济南250100

氢能源作为重要的绿色能源,其制备与应用引起了研究者的极大关注。氨分解在线制氢能够有效解决氢能源储存运输的难题,可以制备得到无碳氧化物杂质的高纯度H_2,但氨分解反应的活化能较高、反应条件苛刻,因此开发高效氨分解催化剂对氢能... 详细信息

氢能源作为重要的绿色能源,其制备与应用引起了研究者的极大关注。氨分解在线制氢能够有效解决氢能源储存运输的难题,可以制备得到无碳氧化物杂质的高纯度H_2,但氨分解反应的活化能较高、反应条件苛刻,因此开发高效氨分解催化剂对氢能源产业发展具有重要意义。稀土氧化物具有较强的表面碱性和良好的热稳定性,其特殊的4f轨道电子结构使其具有储存和释放电子的潜力,易于与活性金属形成结构稳定的界面位点以及增加活性金属的电子密度。因此将稀土材料作为组成部分应用到构建高效稳定的氨分解反应催化剂中具有广阔的研究前景。本文总结了稀土基催化剂催化氨分解反应的进展,对其可以高效促进氨分解反应的内在原因进行了分析,并且对稀土基氨分解催化剂的构效关系揭示和可能的性能优化途径进行了展望。

关键词：氨分解反应稀土基催化剂性能优化构效关系研究

团簇Au/CeO_(2)的制备及其催化CO氧化反应构效关系的研究

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化学学报 2023年第8期81卷 874-883页

作者：付信朴王秀玲王伟伟司锐贾春江山东大学化学与化工学院胶体与界面化学重点实验室特种聚合材料重点实验室济南250100 中山大学材料学院广东深圳518107

负载型Au催化剂因其在诸多反应过程中的高催化活性而备受研究者关注.然而针对负载型催化剂中Au物种结构的有效调控,以及催化过程中真实构-效关系的探索一直充满了挑战.用CeO_(2)为Au物种担载基底,通过简单煅烧处理引起的CeO_(2)结构变化... 详细信息

负载型Au催化剂因其在诸多反应过程中的高催化活性而备受研究者关注.然而针对负载型催化剂中Au物种结构的有效调控,以及催化过程中真实构-效关系的探索一直充满了挑战.用CeO_(2)为Au物种担载基底,通过简单煅烧处理引起的CeO_(2)结构变化,进而实现Au/CeO_(2)之间界面作用力的调控.此研究发现Au纳米颗粒中Au0物种具备更为高效的催化室温CO氧化活性,结合多种原位表征分析,其室温条件下催化转化效率更依赖于CO吸附能力.而相比于单原子Au1和纳米Au颗粒,所制备的团簇Au/CeO_(2)催化剂在较高温度(>50℃)展现出优异的催化CO氧化反应性能.随着温度升高,催化剂表界面O参与的MvK反应路径更易发生,因此具有更多表界面活性O物种和Auδ+位点的团簇Au/CeO_(2)催化剂展现出最为优异的催化CO氧化性能.这些发现为高效负载型Au催化剂的制备提供了新思路并深化了对Au/CeO_(2)催化作用机制的理解.

关键词：负载型金催化剂二氧化铈一氧化碳氧化原位表征反应机理

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《分子模拟》教材建设的探索与实践

大学化学 2023年第6期38卷 189-196页

作者：张恒贾春江宋其圣苑世领山东大学化学与化工学院济南250199

教材建设是课程建设的重要一环,本文重点对山东大学分子模拟实验国家一流课程的教材建设情况进行了介绍。从历史与传承、发展与创新、总结与展望三个方面对山东大学化学学科的教材编写历史、国内外分子模拟相关教材的建设情况、《分子... 详细信息

教材建设是课程建设的重要一环,本文重点对山东大学分子模拟实验国家一流课程的教材建设情况进行了介绍。从历史与传承、发展与创新、总结与展望三个方面对山东大学化学学科的教材编写历史、国内外分子模拟相关教材的建设情况、《分子模拟》教材的主要内容和特色之处,以及下一步的修订计划进行了详细介绍,以期对相关教材的编写与修订提供启发与借鉴。

关键词：计算化学分子模拟教材