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学者姓名：邱文革
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Abstract ：
Palladium-catalyzed Suzuki-Miyaura cross-coupling reaction is a powerful route to construct carbon-carbon bonds in fine-chemical synthesis. However, the activation of relatively chemically inert aryl chlorides under mild conditions in this reaction is still a great challenge. Herein, N-doped hollow carbon nanosheet assemblies (HCNAs) were first developed by hydrothermal carbonization of glucose through an in situ self-generating template method, and the corresponding Pd single-atom catalyst (Pd-1/HCNAs) fabricated by a conventional deposition-precipitation method showed superior catalytic activity (TOFs = 499 h(-1)) and high stability for the Suzuki coupling reaction of chlorobenzene under mild condition. Characterizations of transmission electron microscopy, electron paramagnetic resonance spectroscopy, Raman spectra, X-ray absorption spectroscopy, and X-ray photoelectron spectroscopy showed that the high catalytic activity and stability of Pd-1/HCNAs were related with its full positively charged Pd single-atom active sites and the low reducibility of Pd atom due to the strong interaction between Pd atom and the HCNA carrier. Meanwhile, the relative high chlorobenzene and phenylboric acid adsorption and the low affinity to product biphenyl as well as the special three-dimensional structure of Pd-1/HCNAs were also beneficial to improve the catalytic activity.
Keyword ：
Suzuki-Miyaura cross coupling Suzuki-Miyaura cross coupling palladium single-atom catalysts palladium single-atom catalysts hydrothermal carbonization hydrothermal carbonization activation ofaryl chlorides activation ofaryl chlorides N-doped hollow carbon nanosheetassemblies N-doped hollow carbon nanosheetassemblies
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| GB/T 7714 | Chen, Yun , Zhu, Hongtai , Ding, Xinlei et al. Pd Single Atoms on N-Doped Hollow Carbon Nanosheet Assemblies for Suzuki Cross-Coupling Reactions of Aryl Chlorides [J]. | ACS APPLIED NANO MATERIALS , 2024 , 7 (7) : 8063-8073 . |
| MLA | Chen, Yun et al. "Pd Single Atoms on N-Doped Hollow Carbon Nanosheet Assemblies for Suzuki Cross-Coupling Reactions of Aryl Chlorides" . | ACS APPLIED NANO MATERIALS 7 . 7 (2024) : 8063-8073 . |
| APA | Chen, Yun , Zhu, Hongtai , Ding, Xinlei , Wang, Hanyang , Qiu, Wenge , Song, Jianwei et al. Pd Single Atoms on N-Doped Hollow Carbon Nanosheet Assemblies for Suzuki Cross-Coupling Reactions of Aryl Chlorides . | ACS APPLIED NANO MATERIALS , 2024 , 7 (7) , 8063-8073 . |
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Abstract ：
The activation process is a key step in preparing porous carbon. Herein, three kinds of green activators were separately used to successfully prepare N-doped porous carbons through a two-step strategy: hydrothermal carbonization and chemical activation using microcrystalline cellulose as the carbon source and urea as the nitrogen source. Palladium was deposited on these N-doped microcrystalline cellulose-based carbons (NMC-X, where X represents the activator) via a traditional deposition-precipitation method, and the resulting Pd nanoparticle catalysts (Pd/NMC-X) showed high activity in the selective hydrogenation of quinoline under mild conditions, particularly Pd/NMC-ZC (ZC, zinc carbonate), which achieved complete conversion of quinoline within 100 min at 40 degrees C and 4 atm H-2. Characterization results suggest that the high activity of Pd/NMC-ZC is mainly attributed to the special electronic structure of its Pd species, particularly the distribution of valence states and reducibility of Pd and the high hydrogen spillover capacity between Pd and NMC-ZC. The chemical activation by ZC leads to the formation of multiple defect sites on the carbon skeleton, modifying the carbon surface properties to enhance hydrogen spillover. This also provides an excellent environment for Pd nanoparticle anchoring, thus increasing the Pd-support interactions and regulating the electronic structure of Pd.
Keyword ：
N-doped porous carbon N-doped porous carbon palladiumcatalyst palladiumcatalyst hydrothermal carbonization hydrothermal carbonization chemicalactivation chemicalactivation selective hydrogenation of quinoline selective hydrogenation of quinoline
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| GB/T 7714 | Zhou, Binghui , Ding, Xinlei , Chen, Yun et al. Carbon Defects on N-Doped Carbon Promote Catalytic Activity of Pd Nanoparticles for the Selective Hydrogenation of Quinoline [J]. | ACS APPLIED NANO MATERIALS , 2024 , 7 (19) : 22895-22907 . |
| MLA | Zhou, Binghui et al. "Carbon Defects on N-Doped Carbon Promote Catalytic Activity of Pd Nanoparticles for the Selective Hydrogenation of Quinoline" . | ACS APPLIED NANO MATERIALS 7 . 19 (2024) : 22895-22907 . |
| APA | Zhou, Binghui , Ding, Xinlei , Chen, Yun , Wang, Hanyang , Liu, Yadong , Wang, Chengfei et al. Carbon Defects on N-Doped Carbon Promote Catalytic Activity of Pd Nanoparticles for the Selective Hydrogenation of Quinoline . | ACS APPLIED NANO MATERIALS , 2024 , 7 (19) , 22895-22907 . |
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Abstract ：
负载型金属纳米粒子催化剂被广泛应用于化工工业生产中,但由于金属在高温环境中容易烧结而导致催化剂失活,因此提高催化剂的高温热稳定性是多相催化领域的重大挑战.本文概述了金属纳米颗粒的高温烧结机制:纳米粒子迁移-聚集过程(PMC)和Ostwald熟化(OR),讨论了近年来通过增强金属-载体相互作用、调节金属纳米粒子与包裹层之间的界面效应、构建多功能结构等方法在制备抗烧结型金属纳米催化剂方面的研究进展并对其进行总结.
Keyword ：
高温热稳定性 高温热稳定性 烧结 烧结 催化剂工程 催化剂工程 金属纳米粒子 金属纳米粒子
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| GB/T 7714 | 李淑贞 , 张桂臻 , 杨晓栋 et al. 抗烧结型金属纳米催化剂的制备策略 [J]. | 工业催化 , 2023 , 31 (7) : 1-14 . |
| MLA | 李淑贞 et al. "抗烧结型金属纳米催化剂的制备策略" . | 工业催化 31 . 7 (2023) : 1-14 . |
| APA | 李淑贞 , 张桂臻 , 杨晓栋 , 张龙 , 陈戈 , 邱文革 et al. 抗烧结型金属纳米催化剂的制备策略 . | 工业催化 , 2023 , 31 (7) , 1-14 . |
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Abstract ：
In order to reduce the noble metal palladium dosage in the preparation of CL-20 so as to reduce its production cost, several carbon supports were prepared successfully using the hydrothermal carbonization method in the absence or presence of urea using microcrystalline cellulose (MC) as the carbon source, and the corresponding Pd(OH)(2)/C catalysts were fabricated using the deposition-precipitation method, which showed high activity in the debenzylation reaction of hexabenzylhexaazaisowurtzitane (HBIW) and tetraacetyldibenzylhexaazaisowurtzitane (TADB). It was found that all the catalysts showed a high efficiency in the debenzylation of HBIW, indicating that the structure of the used carbon supports had a limited impact on the catalyst performance in this reaction. On the contrary, the activities of the catalysts in the debenzylation of TADB were quite different. The results of the nitrogen sorption isotherm measurement (BET), scanning electron microscope (SEM), scanning transmission electron microscopy (STEM), powder X-ray diffraction (XRD), element analysis and temperature programmed desorption (TPD), as well as X-ray photoelectron spectra (XPS) characterizations of the supports and catalysts, showed that the relatively high activity of Pd/HTC in the debenzylation of TADB was related to the high Pd dispersion and novel mesoporous structure, while the further higher activity and stability of Pd/HTC-N-1:1 in the same reaction were related with its high Pd dispersion, high total oxidized Pd species, and high surface pyridinic N contents as well as the eggshell distribution of Pd species on the support.
Keyword ：
Pd(OH)(2) Pd(OH)(2) hydrogenolytic debenzylation hydrogenolytic debenzylation C catalyst C catalyst nitrogen doping carbon support nitrogen doping carbon support
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| GB/T 7714 | Wang, Yuling , Chen, Yun , Ding, Xinlei et al. Structural Effects of Microcrystalline Cellulose-Derived Carbon Supports on Catalytic Performance of the Pd(OH)(2)/C Catalysts for the Hydrogenolytic Debenzylation of Hexanitrohexaazaisowurtzitane Derivatives [J]. | CATALYSTS , 2023 , 13 (3) . |
| MLA | Wang, Yuling et al. "Structural Effects of Microcrystalline Cellulose-Derived Carbon Supports on Catalytic Performance of the Pd(OH)(2)/C Catalysts for the Hydrogenolytic Debenzylation of Hexanitrohexaazaisowurtzitane Derivatives" . | CATALYSTS 13 . 3 (2023) . |
| APA | Wang, Yuling , Chen, Yun , Ding, Xinlei , Song, Jianwei , Wei, Gaixia , Dai, Hengwei et al. Structural Effects of Microcrystalline Cellulose-Derived Carbon Supports on Catalytic Performance of the Pd(OH)(2)/C Catalysts for the Hydrogenolytic Debenzylation of Hexanitrohexaazaisowurtzitane Derivatives . | CATALYSTS , 2023 , 13 (3) . |
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Abstract ：
N-doped nestlike carbon nanosheets (NCNs-Nx) were prepared successfully by a two-step strategy, namely, the in situ self-assembly hydrothermal synthesis using glucose as the carbon source in the presence of magnesium nitrate and sodium carbonate and the controlled nitrogen doping carbonization using urea as the nitrogen source. The performance of the corresponding Pd/NCNs-Nx catalysts was investigated for the selective hydrogenation of quinolines. The characterization of transmission electron microscopy, nitrogen sorption isotherm measurement, powder X-ray diffraction, X-ray photoelectron spectra, temperature-programmed desorption of pyridine and benzene, and the pyridine adsorption experiments showed that the very high catalytic activities and selectivity of the Pd/NCNs-Nx catalysts were related with the high Pd dispersion and the electronic structure of Pd species as well as the adsorption capacity and the adsorption type of quinoline molecule on the catalyst surface.
Keyword ：
N-doped nestlike carbon nanosheets N-doped nestlike carbon nanosheets quinoline hydrogenation quinoline hydrogenation hydrothermal synthesis hydrothermal synthesis ultrasmall palladium catalyst ultrasmall palladium catalyst
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| GB/T 7714 | Ding, Xinlei , Chen, Yun , Nan, Junping et al. Ultrasmall Palladium Nanoparticles Anchored on N-Doped Nestlike Carbon Nanosheets for Selective Hydrogenation of Quinolines [J]. | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2022 . |
| MLA | Ding, Xinlei et al. "Ultrasmall Palladium Nanoparticles Anchored on N-Doped Nestlike Carbon Nanosheets for Selective Hydrogenation of Quinolines" . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING (2022) . |
| APA | Ding, Xinlei , Chen, Yun , Nan, Junping , Dai, Hengwei , Wang, Yuling , Bai, Guangmei et al. Ultrasmall Palladium Nanoparticles Anchored on N-Doped Nestlike Carbon Nanosheets for Selective Hydrogenation of Quinolines . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2022 . |
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Abstract ：
高温热稳定性的提高是车用三效催化剂目前面临的主要挑战之一。利用原子层沉积技术(ALD)在新鲜Pt/Al_2O_3催化剂上分别沉积了CeO_2、TiO_2和La_2O_3薄层，采用X射线衍射、透射电子显微镜、氮气低温吸附-脱附和氢气程序升温还原等对催化剂的物理化学性质进行表征，研究沉积氧化物薄层对Pt/Al_2O_3催化剂三效催化反应活性和热稳定性的影响。结果表明，沉积CeO_2、TiO_2和La_2O_3薄层可以提高催化剂性能，还能抑制Pt纳米粒子在800℃和10 h老化过程中聚集长大。在CeO_2、TiO_2和La_2O_3修饰的催化剂中，Pt/Al_2O_3@TiO_2催化剂具有最好的三效...
Keyword ：
催化化学 催化化学 Pt/Al_2O_3催化剂 Pt/Al_2O_3催化剂 三效催化活性 三效催化活性 原子层沉积 原子层沉积 金属氧化物层 金属氧化物层 热稳定性 热稳定性
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| GB/T 7714 | 何泽源 , 朱雨菲 , 张桂臻 et al. 原子层沉积金属氧化物层对Pt/Al_2O_3催化剂三效催化活性和热稳定性的影响 [J]. | 工业催化 , 2022 , 30 (06) : 46-52 . |
| MLA | 何泽源 et al. "原子层沉积金属氧化物层对Pt/Al_2O_3催化剂三效催化活性和热稳定性的影响" . | 工业催化 30 . 06 (2022) : 46-52 . |
| APA | 何泽源 , 朱雨菲 , 张桂臻 , 李淑贞 , 杨晓栋 , 邱文革 et al. 原子层沉积金属氧化物层对Pt/Al_2O_3催化剂三效催化活性和热稳定性的影响 . | 工业催化 , 2022 , 30 (06) , 46-52 . |
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Abstract ：
为提高六硝基六氮杂异伍兹烷（CL‑20）合成过程中氢解脱苄催化剂的活性、降低贵金属Pd用量，本研究以葡萄糖酸钠为原料采用球磨/碳化方法制备了炭载体，实验主要探索了葡萄糖酸钠的碳化温度、升温速率及助剂等因素对炭载体结构及相应氢氧化钯碳（Pd（OH）2/C）催化剂在六苄基六氮杂异伍兹烷（HBIW）和四乙酰基二苄基六氮杂异伍兹烷（TADB）氢解脱苄反应中催化活性的影响。采用氮气等温吸附（BET）、扫描电镜（SEM）、透射电镜（TEM）、X‑射线粉末衍射（XRD）、元素分析及程序升温脱附（TPD）对炭载体的孔结构、颗粒形貌、晶相结构、化学组成及表面化学性质进行了表征。结果表明：以葡萄糖酸钠为原料制备炭载体的较佳碳化温度为700 ℃，升温速率为10 ℃·min-1，引入助剂NaHCO3可调变葡萄糖酸钠碳化过程中的膨化程度。在此优化条件下制备的炭载体具有丰富多级孔结构和适量的表面含氧官能团，相应Pd（OH）2/C催化剂在HBIW和TADB氢解脱苄反应中显示出优异催化活性。
Keyword ：
CL‑20 CL‑20 碳化条件 碳化条件 炭载体结构 炭载体结构 氢解脱苄 氢解脱苄 Pd（OH）2/C催化剂 Pd（OH）2/C催化剂
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| GB/T 7714 | 南俊平 , 王瑜凌 , 宋建伟 et al. 炭载体制备条件对Pd（OH）2/C催化剂氢解脱苄性能的影响 [J]. | 含能材料 , 2022 : 1-10 . |
| MLA | 南俊平 et al. "炭载体制备条件对Pd（OH）2/C催化剂氢解脱苄性能的影响" . | 含能材料 (2022) : 1-10 . |
| APA | 南俊平 , 王瑜凌 , 宋建伟 , 卫改霞 , 陈云 , 丁鑫磊 et al. 炭载体制备条件对Pd（OH）2/C催化剂氢解脱苄性能的影响 . | 含能材料 , 2022 , 1-10 . |
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Abstract ：
The influence of the surface chemical properties of the carbon support on the Pd dispersion, activity and stability of Pd(OH)(2)/C catalyst for the hydrogenolytic debenzylation of tetraacetyldibenzylhexaazaisowurtzitane (TADB) was studied in detail. The flowerlike nanosheet carbon material (NSC) was chosen as the pristine support, meanwhile chemical oxidation with nitric acid and physical calcination at 600 degrees C treatments were used to modify its surface properties, which were denoted as NSCox-2 (treated with 20 wt% HNO3) and NSC-600, respectively. The three carbon supports and the corresponding catalysts of Pd/NSC, Pd/NSC-600, and Pd/NSCox-2 were characterized by scanning electron microscope (SEM), transmission electron microscopy (TEM), nitrogen sorption isotherm measurement (BET), powder X-ray diffraction (XRD), Raman spectra, X-ray photoelectron spectra (XPS), temperature-programmed desorption (TPD), temperature-programmed reduction (H-2-TPR), thermogravimetric analysis (TG), and element analysis. The debenzylation activities of Pd/NSC, Pd/NSC-600, and Pd/NSCox-2, as well as the three catalysts after pre-reduction treatment were also evaluated. It was found that the activity and stability of the Pd(OH)(2)/C catalysts in the debenzylation reaction highly depended on the content of surface oxygen-containing groups of the carbon support.
Keyword ：
palladium catalyst palladium catalyst surface oxygen-containing groups surface oxygen-containing groups palladium dispersion palladium dispersion hydrogenolytic debenzylation hydrogenolytic debenzylation
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| GB/T 7714 | Chen, Yun , Ding, Xinlei , Qiu, Wenge et al. Effects of Surface Oxygen-Containing Groups of the Flowerlike Carbon Nanosheets on Palladium Dispersion, Catalytic Activity and Stability in Hydrogenolytic Debenzylation of Tetraacetyldibenzylhexaazaisowurtzitane [J]. | CATALYSTS , 2021 , 11 (4) . |
| MLA | Chen, Yun et al. "Effects of Surface Oxygen-Containing Groups of the Flowerlike Carbon Nanosheets on Palladium Dispersion, Catalytic Activity and Stability in Hydrogenolytic Debenzylation of Tetraacetyldibenzylhexaazaisowurtzitane" . | CATALYSTS 11 . 4 (2021) . |
| APA | Chen, Yun , Ding, Xinlei , Qiu, Wenge , Song, Jianwei , Nan, Junping , Bai, Guangmei et al. Effects of Surface Oxygen-Containing Groups of the Flowerlike Carbon Nanosheets on Palladium Dispersion, Catalytic Activity and Stability in Hydrogenolytic Debenzylation of Tetraacetyldibenzylhexaazaisowurtzitane . | CATALYSTS , 2021 , 11 (4) . |
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Abstract ：
Research on the design, synthesis, and application of metal organic frameworks (MOFs) based on flexible ligands has attracted significant attention in recent years owing to their superior performance in applications such as gas adsorption and molecular separation. In this work, two acs-type MOFs and an Nbo-type MOF derived from three different flexible diisophthalate ligands were solvothermally prepared and structurally characterized by single crystal X-ray diffraction, powder X-ray diffraction, and thermogravimetric analysis. Analyses of the data revealed that the topologies of the MOFs were correlated to the dihedral angle between the phenyl rings in the ligands.
Keyword ：
Nbo-type MOF Nbo-type MOF acs-type MOF acs-type MOF Flexible diisophthalate ligand Flexible diisophthalate ligand
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| GB/T 7714 | Li, Chuanqiang , Liu, Xiang , Qiu, Wenge et al. MOFs with acs and Nbo topologies using flexible diisophthalate ligands: Influence of dihedral angle between phenyl rings on the crystal structure [J]. | INORGANIC CHEMISTRY COMMUNICATIONS , 2021 , 129 . |
| MLA | Li, Chuanqiang et al. "MOFs with acs and Nbo topologies using flexible diisophthalate ligands: Influence of dihedral angle between phenyl rings on the crystal structure" . | INORGANIC CHEMISTRY COMMUNICATIONS 129 (2021) . |
| APA | Li, Chuanqiang , Liu, Xiang , Qiu, Wenge , Zhang, Yangyang , Zheng, Xuxu . MOFs with acs and Nbo topologies using flexible diisophthalate ligands: Influence of dihedral angle between phenyl rings on the crystal structure . | INORGANIC CHEMISTRY COMMUNICATIONS , 2021 , 129 . |
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Abstract ：
The performance of selective catalytic reduction of NO over ceria-titania (Ce-TiOx)-based materials after aging in SO2 atmosphere in the presence and absence of O-2 was investigated, showing that O-2 gave acceleration on the deactivation of the samples for the enhanced SO2 adsorption and sulfation over ceria-based materials. FT-IR and TPD-MS over samples with 10wt%, 50wt% and 90wt% of CeO2 were carried out. The results indicated the poisoning effect of SO2 over Ce-TiOx catalyst for SCR is in accordance with the amount of sulfite or sulfate over Ce-TiOx with a certain percentage of CeO2.
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| GB/T 7714 | Song, Liyun , Zhan, Zongchen , Sun, Xiangli et al. Effect of SO2 treatment in the presence and absence of O-2 over ceria-titania oxides for selective catalytic reduction [J]. | JOURNAL OF MATERIALS SCIENCE , 2020 , 55 (11) : 4570-4577 . |
| MLA | Song, Liyun et al. "Effect of SO2 treatment in the presence and absence of O-2 over ceria-titania oxides for selective catalytic reduction" . | JOURNAL OF MATERIALS SCIENCE 55 . 11 (2020) : 4570-4577 . |
| APA | Song, Liyun , Zhan, Zongchen , Sun, Xiangli , Zhu, Hongtai , Qiu, Wenge , He, Hong et al. Effect of SO2 treatment in the presence and absence of O-2 over ceria-titania oxides for selective catalytic reduction . | JOURNAL OF MATERIALS SCIENCE , 2020 , 55 (11) , 4570-4577 . |
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