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Synthesis of atomically dispersed cationic nickel-confined mesoporous ZSM-48(ANMZ-48)directed by metal complexes in amphiphilic molecules

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Science China Chemistry 2024年第1期67卷 343-350页

作者： Yu Chen Quanzheng Deng Yiru Mao Yuxi Fang Zhihua Cao honggen peng Shunai Che Lu Han School of Chemical Science and Engineering Tongji UniversityShanghai 200092China School of Chemistry and Chemical Engineering Nanchang UniversityNanchang 330031China School of Chemistry and Chemical Engineering Shanghai Jiao Tong UniversityShanghai 200240China School of Resources and Environment Nanchang UniversityNanchang 330031China State Key Laboratory of Metal Matrix Composites Shanghai Key Laboratory for Molecular Engineering of Chiral DrugsShanghai Jiao Tong UniversityShanghai 200240China

The synthesis of mesoporous zeolite-anchored atomically dispersed metal catalysts(ADCs)is a considerable challenge in chemistry and materials *** we report the synthesis of atomically dispersed cationic nickel-confined mesoporous ZSM-48(ANMZ-48)by in situ hydrothermal reaction employing a designed tri-functional metal complex template,by which the triquaternary ammonium groups in the hydrophilic region direct the formation of ZSM-48 zeolite;the aromatic groups in the hydrophobic tail generate the mesopores through π-π stacking;and the complexes formed by nickel ions coordinated with terpyridyl groups generate atomically dispersed Ni2+confined in zeolite frameworks due to the strong sintering resistance generated by the strong coordination *** ANMZ-48 is consisting of stacking of sheet-like ZSM-48 domains connected by multiply crystal twinning sharing the common(011)plane,generating abundant of imbedded mesopores with the uniform thickness of~2.4 nm and with the width of 10-50 *** excellent catalytic activity and stability of ANMZ-48 were also reflected in the dry reforming of methane(DRM)reaction.

关键词： atomically dispersed catalyst mesoporous zeolite ZSM-48 in situ hydrothermal synthesis the dry reforming of methane reaction

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2015-2021年鄱阳湖流域主要城市PM_(2.5)和O_(3)浓度分布特征及疾病负担评估

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环境科学研究 2024年第5期37卷 975-984页

作者：黄庭赵海星陈奕威马宇佳刘军黄珊彭洪根吴代赦南昌大学资源与环境学院江西南昌330031 鹰潭市特色资源综合利用与智能装备开发重点实验室江西鹰潭335099

为研究鄱阳湖流域主要城市(南昌市、九江市和上饶市)PM_(2.5)和O_(3)污染对健康的影响,本文评估了“十四五”期间实现特定浓度目标可能带来的健康效益,分析了2015-2021年各污染物的浓度变化,并运用健康影响函数(HIF)及综合暴露-反应函数... 详细信息

为研究鄱阳湖流域主要城市(南昌市、九江市和上饶市)PM_(2.5)和O_(3)污染对健康的影响,本文评估了“十四五”期间实现特定浓度目标可能带来的健康效益,分析了2015-2021年各污染物的浓度变化,并运用健康影响函数(HIF)及综合暴露-反应函数(IER)对这些城市的疾病负担进行了评估.结果表明:①2015-2021年,南昌市、九江市和上饶市的PM_(2.5)年均浓度分别下降了28.57%、32.65%和34.88%,而O_(3)浓度分别上升了11.53%、8.75%和7.06%;此外,PM_(2.5)和O_(3)浓度分布呈现出明显的季节性变化.鄱阳湖流域主要城市与PM_(2.5)相关的疾病负担下降了18.42%,而与O_(3)相关的疾病负担增加了81.11%.②预测显示,“十四五”期间若实现积极目标,南昌市、九江市和上饶市的PM_(2.5)疾病负担将分别减少55.45%、59.51%和51.44%,在一般目标下将分别减少31.76%、36.43%和33.80%;O_(3)方面,预期目标实现后南昌市、九江市和上饶市的疾病负担将分别下降50.92%、40.58%和36.80%.研究显示,相较于O_(3)浓度控制目标,更为严格的PM_(2.5)浓度控制目标能够产生更显著的健康效益.

关键词：鄱阳湖流域细颗粒物(PM_(2.5)) 臭氧(O_(3)) 健康影响

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Recent advances in charge mechanism of noble metal-based cathodes for Li-O_(2) batteries

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Chinese Chemical Letters 2023年第2期34卷 109-115页

作者： Yong Zhao Wei Cheng Jiahan Wu Zhengguang Hu Fengliang Liu Li Wang honggen peng Department of Physics Nanchang UniversityNanchang 330031China Xiang Yang Public Inspection and Testing Center Xiangyang 441000China Institute for Advanced Study Nanchang UniversityNanchang 330031China Key Laboratory of Poyang Lake Environment and Resource Utilization Ministry of EducationSchool of Resources Environmental and Chemical EngineeringNanchang UniversityNanchang 330031China

Lithium-oxygen(Li-O_(2)) batteries are considered as the next generation for energy storages systems due to the higher theoretical energy density than that of Li-ion batteries. However, the high charge overpotential caused by the insulated Li_(2)O_(2)results in low energy efficiency, side reaction from electrolyte and cathode, and therefore poor battery performance. Designing noble metal-based catalysts can be an effective strategy to develop high-performance Li-O_(2)batteries with low charge overpotentials and outstanding cycle stability. However, the charge mechanism for noble metal-based catalysts is not clear and even contradictory. Herein, several charge mechanisms of Li_(2)O_(2)are first discussed. Subsequently, the possible charge processes of Li-O_(2)batteries with noble metal-based catalysts are illustrated. In addition, the future development for noble metal-based catalysts is outlined.

关键词： Li-O_(2)batteries Noble metals Charge overpotentials Adsorption energy

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Confined Ni-In intermetallic alloy nanocatalyst with excellent coking resistance for methane dry reforming

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Journal of Energy Chemistry 2022年第2期31卷 34-47页

作者： Wenming Liu Le Li Sixue Lin Yiwei Luo Zhenghong Bao Yiru Mao Kongzhai Li Daishe Wu honggen peng College of Chemistry Key Laboratory of Poyang Lake Environment and Resource UtilizationMinistry of EducationSchool of Resources Environmental and Chemical EngineeringNanchang UniversityNanchang 330031JiangxiChina Chemical Sciences Divison Oak Ridge National LaboratoryOak RidgeTN 37830USA State Key Laboratory of Complex Nonferrous Metal Resources Clean Utilization Engineering Kunming University of Science and TechnologyKunming 650093YunnanChina

Carbon dioxide and methane are two main greenhouse gases which are contributed to serious global ***,dry reforming of methane(DRM),a very important reaction developed decades ago,can convert these two major greenhouse gases into value-added syngas or *** main problem retarding its industrialization is the seriously coking formation upon the nickel-based ***,a series of confined indium-nickel(In-Ni)intermetallic alloy nanocatalysts(In_(x)Ni@SiO_(2))have been prepared and displayed superior coking resistance for DRM *** sample containing 0.5 wt.%of In loading(In_(0.5)Ni@SiO_(2))shows the best balance of carbon deposition resistance and DRM reactivity even after 430 h long term stability *** boosted carbon resistance can be ascribed to the confinement of core–shell structure and to the transfer of electrons from Indium to Nickel in In-Ni intermetallic alloys due to the smaller electronegativity of *** the silica shell and the increase of electron cloud density on metallic Ni can weaken the ability of Ni to activate C–H bond and decrease the deep cracking process of *** reaction over the confined InNi intermetallic alloy nanocatalyst was conformed to the Langmuir-Hinshelwood(L-H)mechanism revealed by in situ diffuse reflectance infrared Fourier transform spectroscopy(in-situ DRIFTS).This work provides a guidance to design high performance coking resistance catalysts for methane dry reforming to efficiently utilize these two main greenhouse gases.

关键词： Methane dry reforming InNi intermetallic alloy Confinement Coking resistance Utilization of greenhouse gases

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Methane dry reforming on Ni/La_2Zr_2O_7 treated by plasma in different atmospheres

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Journal of Energy Chemistry 2015年第4期24卷 416-424页

作者： honggen peng Youhe Ma Wenming Liu Xianglan Xu Xiuzhong Fang Jie Lian Xiang Wang Changqing Li Wufeng Zhou Ping Yuan College of Chemistry Nanchang University Jiangxi Golden Century Advanced Materials Co. Ltd.

A series of Ni/La2Zr2O7 pyrochlore catalysts prepared by impregnation method and treated by dielectric barrier discharge（DBD） plasma in different atmospheres and varied sequences were prepared and applied for dry reforming of methane（DRM）. It is found that all of the plasma treated catalysts show evidently improved activity and coke resistance in comparison with the non-plasma treated one. The best performance is achieved on Ni/La2Zr2O7–H2P–C,a catalyst treated in H2 plasma before calcination. TGA-DSC and SEM demonstrate that carbon deposition is significantly suppressed on all of the plasma treated samples. Moreover,XRD and TEM results testify that both Ni O and Ni sizes on the calcined and reduced samples treated by plasma are also decreased,which results in higher Ni metal dispersion on the reduced and used catalysts and enhances the interactions between Ni sites and the support. It is believed that these are the inherent reasons accounting for the promotional effects of plasma treatment on the reaction performance of the Ni/La2Zr2O7 pyrochlore catalysts.

关键词： Methane dry reforming Ni-based catalysts Pyrochlore support DBD plasma Coke resistance

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Simple nucleophile/H_(2)O promoted defluorinative ring-opening of gem-difluorocyclopropenes

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Green Synthesis and Catalysis 2024年第1期5卷 14-19页

作者： Yimiao He Jingwen Yuan Wen-Xin Lv peng Liu Fan Teng Qijin Mo Zihua Wu Chusheng Huang Qianwen Liu honggen Wang Guangxi Key Laboratory of Natural Polymer Chemistry and Physics College of Chemistry and MaterialsNanning Normal UniversityNanning530001China School of Pharmaceutical Sciences Sun Yat-sen UniversityGuangzhou510006China School of Chemistry Chemical Engineeringand BiotechnologyNanyang Technological University117543Singapore Guangzhou Institutes of Biomedicine and Health Chinese Academy of SciencesGuangzhou510530China Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle Nanchang Hangkong UniversityNanchang330063China

A novel defluorinative ring-opening of gem-difluorocyclopropenes is presented,providing a concise and efficient method for accessing 2-fluoropropenals and 2-fluorobuta-1,3-dienes in moderate to good yields with excellent regio-and *** reaction is performed under mild conditions with no need of using an excess amount of nucleophilic *** plays a crucial role in this transformation.

关键词： gem-difluorocyclopropene Ring-opening defluorination 2-Fluoropropenal 2-Fluorobuta-1,3-diene Water

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Rh(OH)_x/TS-1@KCC-1双功能催化剂上一锅反应合成伯酰胺(英文)

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催化学报 2013年第11期34卷 2057-2065页

作者：彭洪根王达锐徐乐吴鹏华东师范大学化学系上海市绿色化学与化工过程绿色化重点实验室上海200062

在微乳液体系中成功地将花瓣状介孔氧化硅微球(KCC-1)包覆在钛硅分子筛TS-1表面,得到了一种新型微孔/介孔复合核壳结构材料TS-1@KCC-1.详细考察了TS-1@KCC-1的合成条件及可能的形成机理.适宜的合成温度及时间分别为373–393 K和4h.壳层... 详细信息

在微乳液体系中成功地将花瓣状介孔氧化硅微球(KCC-1)包覆在钛硅分子筛TS-1表面,得到了一种新型微孔/介孔复合核壳结构材料TS-1@KCC-1.详细考察了TS-1@KCC-1的合成条件及可能的形成机理.适宜的合成温度及时间分别为373–393 K和4h.壳层厚度可方便地通过改变硅源正硅酸乙酯和TS-1的比例在25–80 nm间进行调控.以TS-1@KCC-1为载体负载Rh(OH)x后即得到双功能催化材料Rh(OH)x/TS-1@KCC-1,该材料同时具有Ti和Rh(OH)x活性中心,可以高效催化醛、氨水和过氧化氢经一锅串联反应直接制备得到伯酰胺.

关键词： TS-1分子筛核壳材料 KCC-1 伯酰胺串联催化剂

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The Application of SnO2-based Catalysts for Emission Control

The Application of SnO2-based Catalysts for Emission Control

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2015年第十四届全国应用化学年会

作者： WANG Xiang peng honggen XU Xianglan peng Yue LI Yarong TIAN Jinshu College of Chemistry Nanchang University

Tetragonal rutile SnO is an n-type semiconductor with a high melting point of 1630℃, thus possessing excellent thermal stability. In addition, it contains abundant surface deficient oxygen species and its lattice oxygen species is also reducible. Therefore, SnO is a potential catalytic material for air emission control reactions. Over the past decades, while its properties as gas sensor or electrode materials have been extensively investigated, its catalytic properties have been much less profiled. Our previous work has demonstrated that SnO-based fine powder catalysts modified by different rare earth metal oxides show much improved thermal stability as well as CO and CH oxidation activity [1]. Moreover, with various simple and feasible methods, pure SnO nano-rod, nano-sheet, nano-needle and hollow sphere samples have also been successfully synthesized, which show reasonable activity and stability for different air emission control reactions [2,3].It is particularly noted here that although pure SnO nano-rod possesses extremely low surface area(1 m/g) and lacks any active oxygen species, it shows much improved CO oxidation activity in comparison with regular SnO powder, due to the presence of preferentially exposed(110) active facets. With the expectation to achieve applicable catalysts for real emission control processes, in this study, several metal cations, such as Mn, Ce and Cu, have been selected to incorporate into the lattice of SnO nano-rod to further improve the activity of the obtained catalysts. As shown by Fig. 1, all the modified samples have the rod-like morphology. XRD results prove that all the different cations have been introduced into the lattice matrix of SnO to form solid solution structure. Compared with pure SnO nano-rod, all the modified nano-rod catalysts display significantly improved CO oxidation activity, as shown by Fig. 2.

关键词： Morphology Controllable Synthesis Nano-rod,Nano-sheet CO Oxidation NOx Selective Reduction

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KCC-1 as a Superior Support to Prepare Catalysts for Air Emission Control and Hydrogen Production

KCC-1 as a Superior Support to Prepare Catalysts for Air Emi...

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中国化学会第九届全国无机化学学术会议

作者： Xiang Wang honggen peng Xianglan Xu Xiuzhong Fang Jiawei Ying Yue peng College of Chemistry Nanchang University

For supported metal catalysts for various reactions, the grain sizes of the active metals and the metal surface areas influence the reaction activity significantly. If a supported active metal has smaller grain sizes and higher dispersion, the prepared catalyst generally possesses better activity [1]. Moreover, in the case of hydrocarbon reforming to produce hydrogen, the smaller Ni size below 5 nm improves not only the activity, but also enhances the coke resistance of a catalyst [2]. Therefore, preparing supported metal catalysts with high metal dispersion and small metal grain size have been a hot research topic and widely explored with different methods. Over the past three years, our research group has been doing a series of systematic work to synthesize high surface area and mesoporous silica supports with different structures and morphologies, which are employed to support various metals such as Pt, Pd, Ni, Cu, Pt-Ni, Pd-Ni and Pt-Cu alloys to prepare catalysts for CO, CH4 and VOCs oxidation, NOx selective reduction and low hydrocarbon reforming for hydrogen production. Among all of the mesoporous Si O2(SBA-15, MCM-41 and KCC-1) prepared in this lab, it is found that dendritic silica nano-sphere(KCC-1) [3] is a superior support to prepare Pt and Pt-Ni/KCC-1 for CO oxidation, Cu/KCC-1 for CO oxidation and NOx reduction and Ni/KCC-1 for hydrocarbon reforming for hydrogen production. Due to the high surface area, the fibrous morphology and the presence of a large amount of mesopores(Fig. 1), the dispersion of the supported metals is greatly improved, and the mobilization of the supported metals at high temperature has been effectively impeded. As a consequence, more active and stable catalysts for both of emission control and hydrogen production reactions have been achieved.

关键词： Mesoporous silica KCC-1 CO oxidation NOx Selective Reduction Hydrogen Production

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合成超小MOR型分子筛纳米颗粒（英文）

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Science China Materials 2018年第9期61卷 1185-1190页

作者：许义申学峰彭程马跃韩璐吴鹏彭洪根车顺爱 School of Chemistry and Chemical Engineering State Key Laboratory of Metal Matri Composites Shanghai Jiao Tong University Institute of Applied Chemistry College of Chemistry Nanchang University Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular Engineering East China Normal University School of Chemical Science and Engineering Tongji University

本文在一个较低的温度(403 K)下使用四乙基溴化铵(TEAB)为模板剂合成出超小的(30 nm)MOR型分子筛.超小的产物粒径是由于高浓度的TEAB可以提供更多的晶核以及低温限制了奥氏熟化.产物在低温区域的NO_x选择性催化还原活性远远高于传统MOR... 详细信息

本文在一个较低的温度(403 K)下使用四乙基溴化铵(TEAB)为模板剂合成出超小的(30 nm)MOR型分子筛.超小的产物粒径是由于高浓度的TEAB可以提供更多的晶核以及低温限制了奥氏熟化.产物在低温区域的NO_x选择性催化还原活性远远高于传统MOR型分子筛.此外,超小的纳米颗粒减小了物质的传输限制以及较大的比表面积使得其在甲苯歧化反应中具有比传统MOR更高的催化活性和耐失活性.

关键词：纳米颗粒分子筛 MOR R型合成催化还原活性四乙基溴化铵催化活性

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