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Single-atom Pd anchored in the porphyrin-center of ultrathin 2D-MOFs as the active center to enhance photocatalytic hydrogen-evolution and NO-removal

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Chinese Chemical Letters 2024年第9期35卷 364-368页

作者： Xingyan Liu Chaogang Jia Guangmei Jiang chenghua zhang Mingzuo Chen Xiaofei Zhao Xiaocheng zhang Min Fu Siqi Li Jie Wu Yiming Jia Youzhou He Chongqing Key Laboratory of Catalysis and New Environmental Materials College of Environment and ResourcesChongqing Technology and Business UniversityChongqing 400067China School of Pharmacy North Sichuan Medical CollegeNanchong 637100China Carbon Neutrality Technology Application Research Center College of River and Ocean EngineeringChongqing Jiaotong UniversityChongqing 400074China State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China National Local Joint Engineering Research Center for Road Engineering and Disaster Prevention and Reduction Technology in Mountainous Areas China Merchants Chongqing Communications Technology Research and Design Institute Co.Ltd.Chongqing 400067China Chongqing Culture Relics and Archaeology Research Institute Chongqing 400013China

Single-atom catalysts were widely used to treat atmospheric pollution and alleviate energy crises through ***,how to prevent the aggregation of single atoms during the preparation and catalytic processes remained a great ***,a novel ultrathin two-dimensional porphyrin-based single-atom photocatalyst Ti-MOF(abbreviated as TMPd)obtained through a simple hydrothermal synthesis strategy was used for photocatalytic hydrogen evolution and NO removal,in which the singleatom Pd tightly anchored in the center of porphyrin to ensure single-atom Pd stable *** with most reported MOFs-based photocatalysts,the TMPd showed an excellent hydrogen evolution rate(1.32 mmol g^(-1)h^(-1))and the NO removal efficiency(62%)under visible light *** high-angle annular dark-field scanning transmission electron microscope(HAADF-STEM)and synchrotron-radiation-based X-ray absorption fine-structure spectroscopy(XAFS)proved that pd in TMPd existed in an isolated state,and the atomic force microscope(AFM)proved the ultrathin morphology of *** calculations had demonstrated that single-atom Pd could serve as the active center and more effectively achieve electron transfer,indicating that single-atom Pd played a vital role in photocatalytic hydrogen *** addition,a possible photocatalytic pathway of NO removal was proposed based on ESR and in-situ infrared spectra,in which the catalysts anchored with single-atom Pd could produce more active substances and more effectively oxidize NO to NO_(2)^(-)or NO_(3)^(-).The results suggested that coordinating single-atom metal species as the active site in the center of porphyrin could be a feasible strategy to obtain various ultrathin porphyrin-based single-atom photocatalysts to acquire excellent photocatalytic performance further.

关键词： Porphyrin-based MOFs Single-atom Pd Ultrathin 2D nanosheets Hydrogen evolution NO removal

In-situ fabrication of TiO_(2)/NH_(2)-MIL-125(Ti) via MOF-driven strategy to promote efficient interfacial effects for enhancing photocatalytic NO removal activity

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Chinese Chemical Letters 2024年第10期35卷 389-393页

作者： Maosen Xu Pengfei Zhu Qinghong Cai Meichun Bu chenghua zhang Hong Wu Youzhou He Min Fu Siqi Li Xingyan Liu Chongqing Key Laboratory of Catalysis and New Environmental Materials College of Environment and ResourcesChongqing Technology and Business UniversityChongqing400067China School of Pharmacy North Sichuan Medical CollegeNanchong 637100China State Key Joint Laboratory of Environment Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China

Deep oxidation of NO molecules to nitrate species by photocatalysis with virtually no toxic byproduct NO_(2)generation is a challenging *** this study,Ti O_(2)in-situ grows based on NH_(2)-MIL-125(Ti)(NM-125)not only inhibited TiO 2agglomeration,but also contacted more tightly to obtain efficient interfacial effects,thus displaying excellent photocatalytic NO removal activity(68.08%).The formation of Ti O_(2) is directly confirmed by characterizations such as X-ray diffraction(XRD),transmission electron microscope(TEM),X-ray photoelectron spectroscopy(XPS).Meanwhile,UV–vis,photoluminescence,and photoelectrochemical analysis indicate that TiO_(2) formation effectively improves the optical ***,the strong electron interaction and electron transport direction between NM-125 and Ti O_(2) are investigated by density functional theoretical(DFT)***,combined with the results of electron spin resonance(ESR)and in-situ FT-IR test,the intermediate processes of NO adsorption and photocatalytic oxidation reaction are discussed in depth,where the production of reactive oxygen species(ROS)under light is the key factor in the successful degradation of *** with NM-125 which can only produce·OH through photogenerated electrons since the lower valence band position,NMT-2 can directly produce·OH through photogenerated holes,thereby relieving the pressure on photogenerated electrons and producing more *** study will provide reasonable guidance for the modification of NM-125 for photocatalytic removal of ppb-level NO.

关键词： Photocatalysis NH_(2)-MIL-125(Ti) TiO_(2) No removal ROS

“两个结合”引领当代中国文学批评实践——中国文学批评研究会2023年年会暨“两个结合与文学批评的使命”学术研讨会综述

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中国文学批评 2024年第2期 186-188,192页

作者：张成华华南师范大学文学院广州510006

2021年7月1日,习近平总书记在庆祝中国共产党成立100周年大会上的讲话中提出,“坚持把马克思主义基本原理同中国具体实际相结合、同中华优秀传统文化相结合”。在党的二十大报告中,习近平总书记进一步阐明了“两个结合”的基本内涵和实... 详细信息

2021年7月1日,习近平总书记在庆祝中国共产党成立100周年大会上的讲话中提出,“坚持把马克思主义基本原理同中国具体实际相结合、同中华优秀传统文化相结合”。在党的二十大报告中,习近平总书记进一步阐明了“两个结合”的基本内涵和实践意义。为深入领会和贯彻习近平总书记“两个结合”的丰富内涵和精髓要义,总结中国文学批评的历史经验。

关键词：中国文学批评文学批评实践中华优秀传统文化马克思主义基本原理基本内涵丰富内涵实践意义

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Fe/BN催化剂的制备及其费托合成性能

低碳化学与化工 2024年第2期49卷 26-34页

作者：王宪周张成华相宏伟中国石油化工股份有限公司石油化工科学研究院北京100083 中国石油化工股份有限公司茂名分公司广东茂名525000 安徽大学化学化工学院安徽合肥230601 中国科学院山西煤炭化学研究所煤炭高效低碳利用全国重点实验室山西太原030001

为开发基于高热传导性载体的催化剂,提高费托合成反应性能,以高比表面积的球磨氮化硼(BN)为载体,通过溶剂热法(溶剂热温度分别为120℃、160℃和200℃)制备了系列Fe/BN催化剂(Fe/BN-120、Fe/BN-160和Fe/BN-200),并研究了催化剂对费托合... 详细信息

为开发基于高热传导性载体的催化剂,提高费托合成反应性能,以高比表面积的球磨氮化硼(BN)为载体,通过溶剂热法(溶剂热温度分别为120℃、160℃和200℃)制备了系列Fe/BN催化剂(Fe/BN-120、Fe/BN-160和Fe/BN-200),并研究了催化剂对费托合成的催化性能(温度为280℃、压力为2.0 MPa、合成气V(H2):V(CO):V(Ar)=16:8:1且空速为3000 mL/(g·h),以48h时的反应结果计)。采用N_(2)吸/脱附、电感耦合等离子体-原子发射光谱(ICP-AES)、X-射线衍射(XRD)、透射电子显微镜(TEM)、X-射线电子能谱(XPS)和H_(2)/CO程序升温还原(H_(2)/CO-TPR)等对催化剂进行了表征。结果表明,与Fe/BN-120相比,Fe/BN-160、Fe/BN-200中γ-Fe_(2)O_(3)的平均粒径分别由7.2 nm增加至13.6 nm、14.7 nm,同时Fe 2p结合能逐渐向低结合能方向偏移。与Fe/BN-120和Fe/BN-160相比,在电子效应和尺寸效应的作用下,Fe/BN-200的还原、碳化得到明显促进。在费托合成的CO_(2)和H_(2)O气氛中,还原得到的α-Fe、Fe_(3)O_(4)和球磨氮化硼表面的BOx在高温条件下发生反应生成硼酸铁。随着溶剂热温度的升高,催化剂的碳化程度逐渐升高,与Fe/BN-120相比(CO转化率为39.1%、CH_(4)选择性为24.3%和C_(5+)选择性为37.8%),Fe/BN-200的CO转化率提高至68.9%,CH_(4)选择性降至12.9%,C_(5+)选择性增加至51.1%。在Fe/BN催化剂上,通过改变溶剂热温度可以调控催化活性和产物分布,这为提高氮化硼负载的Fe基催化剂的费托合成反应性能提供了思路。

关键词：费托合成铁基催化剂氮化硼溶剂热法催化活性

Comparison of the level of thrombus precursor protein in blood plasma between patients with acute cerebral infarction and healthy persons at different time

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Neural Regeneration Research 2006年第3期1卷 258-260页

作者： chenghua Xiao Peng zhang Department of Neurology Affiliated Hospital of Xuzhou Medical College Xuzhou 221002 Jiangsu Province China

BACKGROUND： Thrombus precursor protein （TpP） is the index of thrombus activity level, and it is also early referencing index in detecting thrombus diseases. OBJECTIVE： To dynamically observe the changes of TpP level in blood plasma of patients with acute cerebral infarction at different time after onset, and to compare the differences of plasma TpP level between patients with acute cerebral infarction and healthy persons who received health examination. DESIGN： Controlled observation SETTING： Department of Neurology, Affiliated Hospital of Xuzhou Medical College PARTICIPANTS： Totally 58 patients with acute cerebral infarction who received the treatment in the Department of Neurology, Affiliated Hospital of Xuzhou Medical College between September 2004 and March 2005 were recruited in this study. They all met the diagnostic criteria revised by the 4^th National Conference of Cerebrovascular Disorders in 1995 and were diagnosed by clinical and skull CT and （or） MRI examinations. The patients included 33 male and 25 female aged from 36 to 87 years. Time to onset 〈 6 hours, 6 to 11 hours, 12 to 23 hours, 24 to 48 hours and 〉 48 hours were found in 10,11,14,10 and 13 patients respectively. Another 51 persons who homeochronously received the health body examination in our hospital were recruited, including 34 male and 17 female, aged 38 to 85 years, serving as control group. Patients with cardio-cerebrovascualr diseases or liver and kidney diseases were excluded. All the involved subjects were informed of the detected items. METHODS： About 4 mL venous blood was respectively taken from patients admitted to the hospital within 6 hours, 6 toll hours, 12 to 23 hours, 24 to 48 hours and more then 48 hours after onset, and healthy persons when receiving health examination. The level of TpP in blood plasma was measured with enzymelinked immunosorbent assay. MAIN OUTCOME MEASURES： ① Comparison of the level of plasma TpP between patients and controls;② Comparison of the level of p

关键词： Comparison of the level of thrombus precursor protein in blood plasma between patients with acute cerebral infarction and healthy persons at different time time

高分散Ru/Si_(3)N_(4)催化剂的制备及其在CO_(2)加氢中的应用

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低碳化学与化工 2024年第3期49卷 9-17页

作者：颜琳琳魏宇学张成华相宏伟李永旺中石化石油化工科学研究院有限公司北京100083 中国石油化工股份有限公司茂名分公司广东茂名525000 安徽大学化学化工学院安徽合肥230601 中科合成油技术股份有限公司国家能源煤基液体燃料研发中心北京101407 中国科学院山西煤炭化学研究所煤炭高效低碳利用全国重点实验室山西太原030001

氮化硅是一种良好的载体,具有较高的水热稳定性和机械稳定性,其表面的氨基基团能够较好地锚定金属,显著提高金属分散度。但是,商品氮化硅比表面积较低,对金属分散作用仍然有限。因此,以自制的高比表面积氮化硅(Si_(3)N_(4))为载体,通过... 详细信息

氮化硅是一种良好的载体,具有较高的水热稳定性和机械稳定性,其表面的氨基基团能够较好地锚定金属,显著提高金属分散度。但是,商品氮化硅比表面积较低,对金属分散作用仍然有限。因此,以自制的高比表面积氮化硅(Si_(3)N_(4))为载体,通过浸渍法制备了不同Ru负载量(质量分数分别为0.5%、1.0%和2.0%)的催化剂(分别为0.5%Ru/Si_(3)N_(4)、1.0%Ru/Si_(3)N_(4)和2.0%Ru/Si_(3)N_(4)),并以商品氮化硅(Si_(3)N_(4)-C)为载体制备了2.0%Ru/Si_(3)N_(4)-C催化剂作为对照组。表征了催化剂的理化性质,测试了其在300℃、0.1 MPa下的CO_(2)加氢反应活性。结果显示,与Si_(3)N_(4)-C相比,Si_(3)N_(4)的比表面积较高(502 m^(2)/g),Si_(3)N_(4)作为载体显著提高了金属分散度,降低了金属粒径,催化剂暴露出更多的活性位点。0.5%Ru/Si_(3)N_(4)的金属粒径较小,展现出强的H_(2)吸附能力,H难以解吸,抑制了中间物种CO加氢生成CH_(4)。随着Ru负载量增加,金属粒径增大,催化剂的CH_(4)选择性更好。Ru/Si_(3)N_(4)系列催化剂中,2.0%Ru/Si_(3)N_(4)的CH_(4)选择性较高(98.8%)。空速为10000 m L/(g·h)时,0.5%Ru/Si_(3)N_(4)的CO选择性为88.2%。与2.0%Ru/Si_(3)N_(4)相比,2.0%Ru/Si_(3)N_(4)-C的金属粒径更大,活性位点较少,活性更低。2.0%Ru/Si_(3)N_(4)和2.0%Ru/Si_(3)N_(4)-C的CO_(2)转化率分别为53.1%和9.2%。Si_(3)N_(4)有效提高了金属分散度,提高了催化剂的CO_(2)加氢反应活性;通过调控Ru负载量控制催化剂金属粒径,可实现对产物CO或CH_(4)选择性的调控。

关键词： CO_(2)加氢 Ru/Si_(3)N_(4)催化剂 CH_(4)选择性 CO选择性

Study of Manganese Promoter on a Precipitated Iron-Based Catalyst for Fischer-Tropsch Synthesis

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Journal of Natural Gas Chemistry 2007年第3期16卷 278-285页

作者： Zhichao Tao Yong fang chenghua zhang Tingzhen Li Mingyue Ding Hongwei Xiang Yongwang Li State Key Laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences Taiyuan 030001 Shanxi China Graduate University of Chinese Academy of Sciences Beijing 100039 China

The effects of Manganese （Mn） incorporation on a precipitated iron-based Fischer-Tropsch synthesis （FTS） catalyst were investigated using N2 physical adsorption, air differential thermal analysis （DTA）, H2 temperature-programmed reduction （TPR）, and Mǒssbauer spectroscopy. The FTS performances of the catalysts were tested in a slurry phase reactor. The characterization results indicated that Mn increased the surface area of the catalyst, and improved the dispersion of （α-Fe2O3 and reduced its crystallite size as a result of the high dispersion effect of Mn and the Fe-Mn interaction. The Fe-Mn interaction also suppressed the reduction of （α-Fe2O3 to Fe3O4, stabilized the FeO phase, and （or） decreased the carburization degree of the catalysts in the H2 and syngas reduction processes. In addition, incorporated Mn decreased the initial catalyst activity, but improved the catalyst stability because Mn restrained the reoxidation of iron carbides to Fe3O4, and improved further carburization of the catalysts. Manganese suppressed the formation of CH4 and increased the selectivity to light olefins （C2-4^=）, but it had little effect on the selectivities to heavy （C5＋） hydrocarbons. All these results indicated that the strong Fe-Mn interaction suppressed the chemisorptive effect of the Mn as an electronic promoter, to some extent, in the precipitated iron-manganese catalyst system.

关键词： Fischer-Tropsch synthesis iron-manganese catalyst manganese promoter Fe-Mn interaction

Effect of Sulfate on an Iron Manganese Catalyst for Fischer-Tropsch Synthesis

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Journal of Natural Gas Chemistry 2007年第4期16卷 354-362页

作者： Tingzhen Li Yong Yang Zhichao Tao Haijun Wan Xia An chenghua zhang Hongwei Xiang Yongwang Li State Key Laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences Taiyuan 030001 Shanxi China Graduate University of the Chinese Academy of Sciences Beijing 100029 China

The effect of sulfate on Fischer-Tropsch synthesis performance was investigated in a slurryphase continuously stirred tank reactor （CSTR） over a Fe-Mn catalyst. The physiochemical properties of the catalyst impregnated with different levels of sulfate were characterized by N2 physisorption, X-ray photoelectron spectroscopy （XPS）, H2 （or CO） temperature-programmed reduction （TPR）, Mossbauer spectroscopy, and CO2 temperature-programmed desorption （TPD）. The characterization results indicated that the impregnated sulfate slightly decreased the BET surface area and pore volume of the catalyst, suppressed the catalyst reduction and carburization in CO and syngas, and decreased the catalyst surface basicity. At the same time, the addition of small amounts of sulfate improved the activities of FischerTropsch synthesis （FTS） and water gas shift （WGS）, shifted the product to light hydrocarbons （C1-C11） and suppressed the formation of heavy products （C12＋）. Addition of SO4^2- to the catalyst improved the FTS activity at a sulfur loading of 0.05-0.80 g per 100 g Fe, and S-05 catalyst gave the highest CO conversion （62.3%）, and beyond this sulfur level the activity of the catalyst decreased.

关键词： Fischer-Tropsch synthesis iron-based catalyst sulfate content ferrous sulfate manganese

Effect of Manganese Incorporation Manner on an Iron-Based Catalyst for Fischer-Tropsch Synthesis

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Journal of Natural Gas Chemistry 2007年第3期16卷 244-251页

作者： Tingzhen Li Yong Yang chenghua zhang Zhichao Tao Haijun Wan Xia An Hongwei Xiang Yongwang Li State Key Laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences Taiyuan 030001 Shanxi China Graduate University of the Chinese Academy of Sciences Beijing 100029 China

A systematic study was undertaken to investigate the effects of the manganese incorporation manner on the textural properties, bulk and surface phase compositions, reduction/carburization behaviors, and surface basicity of an iron-based Fischer-Tropsch synthesis （FTS） catalyst. The catalyst samples were characterized by N2 physisorption, X-ray photoelectron spectroscopy （XPS）, H2 （or CO） temperature-programmed reduction （TPR）, CO2 temperature-programmed desorption （TPD）, and M5ssbauer spectroscopy. The FTS performance of the catalysts was studied in a slurry-phase continuously stirred tank reactor （CSTR）. The characterization results indicated that the manganese promoter incorporated by using the coprecipitation method could improve the dispersion of iron oxide, and decrease the size of the iron oxide crystallite. The manganese incorporated with the impregnation method is enriched on the catalyst＇s surface. The manganese promoter added with the impregnation method suppresses the reduction and carburization of the catalyst in H2, CO, and syngas because of the excessive enrichment of manganese on the catalyst surface. The catalyst added manganese using the coprecipitation method has the highest CO conversion （51.9%） and the lowest selectivity for heavy hydrocarbons （C12＋）.

关键词： Fischer-Tropsch synthesis iron-based catalyst manganese promoter incorporation manner