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Molecular Catalysis · 2020 · IF 3.687

Mild-temperature hydrogenation of carbonyls over Co-ZIF-9 derived Co-ZIF-x nanoparticle catalyst

Fanfan Yue,Ao Hu,Xinhuan Lu,Chenlong Wang,Haijun Pan,Haifu Zhang,Lu Yang,Qinghua Xia,Dan Zhou,Yongde Xia

Benzimidazole and metal cobalt salts were employed in the synthesis of Co-ZIF-9 by solvothermal crystallization. Highly active catalysts for selective hydrogenation of carbonyl compounds were developed. The optimal nanocatalyst Co-ZIF-350 manifested remarkable activity and selectivity for the hydrogenation of cyclohexanone under mild conditions. Catalytic conversion of cyclohexanone reached the highest over the catalyst of Co-ZIF-9-pyrolyzed at 350 °C for 2 h, in which the conversion of cyclohexanone was 100 % and the selectivity of cyclohexanol was >99 % at 50 °C. A wide scope of ketones/aromatic aldehydes could be selectively reduced to the corresponding alcohols with high yields. Importantly, the nanocatalyst Co-ZIF-350 presented good tolerance of substrates with various functional groups under mild conditions.

研究领域: 催化化学 · 材料科学
✓ 已验证 DOI 高影响因子
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Green Energy & Environment · 2021 ·Vol. 8 ·期 2 ·589-600 · IF 8.207

Metal organic framework supported niobium pentoxide nanoparticles with exceptional catalytic effect on hydrogen storage behavior of MgH2

Liuting Zhang,Farai Michael Nyahuma,Haoyu Zhang,Changshan Cheng,Jiaguang Zheng,Fuying Wu,Lixin Chen

Nb 2 O 5 nanoparticles with an average particle size of 10 nm supported on a rhombic dodecahedral metal organic framework (MOF) were successfully synthesized by a facile one-pot hydrothermal reaction and subsequent calcination process. Experimental results demonstrated that the prepared catalyst drastically improved the hydrogen storage behavior of MgH 2 . 7 wt% Nb 2 O 5 @MOF doped MgH 2 started to desorb hydrogen at 181.9 °C and 6.2 wt% hydrogen could be released within 2.6 min and 6.3 min at 275 °C and 250 °C, respectively. The fully dehydrogenated composite also displayed excellent hydrogenation by decreasing the onset absorption temperature to 25 °C and taking up 4.9 wt% and 6.5 wt% hydrogen within 6 min at 175 °C and 150 °C, respectively. Moreover, the corresponding activation energy was calculated to be 75.57 ± 4.16 kJ mol −1 for desorption reaction and 51.38 ± 1.09 kJ mol −1 for absorption reaction. After 20 cycles, 0.5 wt% hydrogen capacity was lost for the MgH 2 +7 wt% Nb 2 O 5 @MOF composite, much lower than 1.5 wt% of the MgH 2 +7 wt% Nb 2 O 5 composite. However, the addition of Nb 2 O 5 @MOF had limited effect on reducing the dehydrogenation enthalpy of MgH 2 . Microstructure analysis revealed that Nb 2 O 5 particles were uniformly distributed on surface of the MgH 2 matrix and synergistically improved the hydrogen storage property of MgH 2  with MOF.

研究领域: 材料科学 · 无机化学 · 纳米催化 · 能源存储 · 氢能源 · 固态储氢
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Energy & Environment · 2022 · IF 3.154

Hydrocarbon regulation and lower temperature pyrolysis of balikun oil shale kerogen

Fei Liu,Weiguang Shi,Tianbao Liu,Wei Li,Liang Sun,Xiangbin Liu,Changming Zhao,Benxian Li,Sunhua Deng,Zhaohui Dong,Chengwu Xu,Xiaofei Fu,Xiuling Yan

Oil shale kerogen is a kind of composite nature of fossil energy polymer. Kerogen pyrolysis is a feasible and alternative strategy to produce fossil fuels from shales. However, the disadvantages including the high energy consumption, the high cost, and the low hydrocarbon conversion, significantly hinder the development and utilization of unconventional hydrocarbon resources. Herein, the hexagonal crystal structural layered double hydroxides (LDHs) with the Ni/Fe ratio of 5.64:2.36 is proposed as pyrolysis catalyst to improve the catalytic efficiency, the selectivity of target hydrocarbons, and lower the temperature for the process of kerogen pyrolysis. As a result, needle-like nanoscale NiFe-LDHs are prepared successfully to perform the fast thermal upgrading of Balikun oil shale kerogen. The catalytic pyrolysis performance has been observed that the temperature for maximum conversion (Tmax) is 401.18 °C, presenting a Tmax reduction of 37.84 °C, the yield of shale oil is increased by 7.83 wt%. And during 350°C– 400°C, a progressive increment of 147.67%, 230.86%, and 310.61% is obtained corresponding to the content of C1-C5, C6-C14, and C14 + hydrocarbons, respectively. This finding enriches the catalyst candidates for kerogen pyrolysis and provides new insights into industrial applications of in-situ pyrolysis technology for oil shale recovery processes.

研究领域: 能源化学 · 石油工程 · 材料科学
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ACS Catalysis · 2017 · IF 10.614

TiO2–x-Modified Ni Nanocatalyst with Tunable Metal–Support Interaction for Water–Gas Shift Reaction

Ming Xu,Shan He,Hao Chen,Guoqing Cui,Lirong Zheng,Bin Wang,Min Wei

The modulation of strong metal–support interaction (SMSI) plays a key role and remains a challenge in achieving the desired catalytic performance in many important chemical reactions. Herein, we report a TiO2–x-modified Ni nanocatalyst with tunable Ni–TiO2–x interaction via a two-step procedure: preparation of Ni/Ti mixed metal oxide (NiTi–MMO) from NiTi-layered double hydroxide (NiTi–LDH) precursor, followed by a further reduction treatment at different temperatures. A combination study (XRD, TEM, H2-TPR, XPS, and in situ EXAFS) verifies that a high reduction temperature enhances the Ni–TiO2–x interaction, which results in an increased coverage degree of Ni nanoparticles by TiO2–x as well as electron density of interfacial Ni (Niδ−). Moreover, the creation of a Niδ−–Ov–Ti3+ interface site (Ov denotes oxygen vacancy) induced by strong Ni–TiO2–x interaction serves as dual-active site to efficiently catalyze the water–gas shift reaction (WGSR). The optimized catalyst (Ni@TiO2–x(450)) via tuning Ni–TiO2–x interaction gives a TOF value of 3.8 s–1, which is ∼7 times larger than the conventional 15%Ni/TiO2(450) catalyst. Such a high catalytic efficiency is attributed to the interfacial site (Niδ−–Ov–Ti3+) with medium strength of metal–support interaction, as revealed by in situ diffuse reflectance Fourier transform infrared spectroscopy (in situ DRIFTS), which promotes the synergic catalysis between Niδ− and oxygen vacancy toward WGSR.

研究领域: 催化化学 · 材料科学 · 表面科学 · 能源化学 · 纳米催化
✓ 已验证 DOI 高影响因子
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2024 · IF 8.1

Perovskiet-like BaZrO3 nanocatalyst with rich oxygen vacancies on boosting hydrogen storage property of MgH2

Chenxi Liang,Yan Fan,Zhenbin Wang,Yongquan Zhou,Mingjin Zhang,Cunhua Ma

Magnesium hydride (MgH 2 ) as a promising solid hydrogen syorage material has been extensively researched. but the higher separating temperature and sluggish kinetics hinder its large-scale practical application. To solve this problem, a BaZrO 3 nanocatalyst with abundant oxygen vancies is manuscripted, exerts significant improvement to the hydrogen storage performance of MgH 2 . Impressively, the onset dehydrogenation temperature of MgH 2 -10 wt% BaZrO 3 -O v composite is reduced markedly from 390 °C(for pure MgH 2 ) to 260 °C. Additionally, the composite can discharge 4.22 wt% H 2 with 10 min at 275 °C and a total dehydrogenation amouut of 5.88 wt% is achieved at 300 °C. For hydrogen absorption, the composite can rapidly recharge hydrogen at a low temperature of 150 °C and approximately 5.08 wt% H 2 can be absorbed at 275 °C within 10 min. The dehydrogenation activation energy of BaZrO 3 -O v -added MgH 2 is as low as 92.61 kJ mol −1 compared to pure MgH 2 (164.78 kJ mol −1 ). Meantime, the composite presents unexceptionable reversible kinetic performance with a retention rate of 97.35 % after 10 cycles. The excellent catalytic effects can be attributed to the in-situ generation of ZrO 2 -O v , BaO-O v and ZrH 2 from BaZrO 3 -O v during the first de-/rehydrogenation cycle, which function as nanosized active sites on MgH 2 matrix to accelerate electron transfer and provide abundant hydrogen diffusion channels. Density functional theory calculations results verify that the Mg–H length and dehydrogenation energy barrier are ameliorated through BaZrO 3 -O v . This work provides a unique perspective on modification MgH 2 by perovskiet-like BaZrO 3 -O v nanocatalyst.

研究领域: 材料科学 · 氢气储存 · 纳米催化 · 能源材料
✓ 已验证 DOI 高影响因子
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WATER SCIENCE AND TECHNOLOGY · 2022 ·Vol. 85 ·期 4 ·1235-1249 · IF 2.43

Insight into the performance and mechanism of magnetic Ni0.5Cu0.5Fe2O4 in activating peroxydisulfate for ciprofloxacin degradation

Wang Bo,Li Shifeng,Wang Haibo,Yao Shuhua

Magnetic nickel-copper ferrite (Ni x Cu y Fe 2 O 4 ) nano-catalyst was synthesized by co-precipitation method, and it exhibited excellent ability for activating peroxydisulfate (PDS) in the degradation of ciprofloxacin (CIP). As-prepared Ni 0.5 Cu 0.5 Fe 2 O 4 properties were characterized by Fourier-transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), scanning electron microscope equipped with an energy-dispersive X-ray (SEM-EDX), transmissions electron microscopy (TEM), N 2 adsorption-desorption isotherm plot of Brunauer-Emmett-Teller (BET) and Barrett-Joyner-Halenda (BJH), vibrating sample magnetometer (VSM). The maximum degradation efficiency is 80.2% by using 0.500 g/L of Ni 0.5 Cu 0.5 Fe 2 O 4 for activating 5.00 mmol/L of PDS to degrade CIP (20.0 mg/L) at 25 ± 2 °C for 50 min (pH = 6.00). The presence of interfering ions Cl − , NO 3 − , and HCO 3 − inhibited the reaction by producing reactive species with low oxidation potential, inducing the degradation efficiency down to 60.0%, 58.1% and 21.5% respectively. Ni 0.5 Cu 0.5 Fe 2 O 4 displayed great magnetic separation characteristic for the satisfactory magnetization; saturation value is ∼8.6 emu/g. The degradation efficiency of recycled samples has no significant difference after using three times, which is about 60%, indicating that Ni 0.5 Cu 0.5 Fe 2 O 4 is a reusability catalyst in activating PDS for CIP degradation. This work might provide an efficient and promising approach to construct recyclable magnetic materials that can be used for wastewater treatment. Magnetic nano-catalyst was synthesized via co-precipitation. Ni 0.5 Cu 0.5 Fe 2 O 4 displayed excellent ability in activating peroxydisulfate. Ni 0.5 Cu 0.5 Fe 2 O 4 displayed great magnetic separation characteristic. Ni 0.5 Cu 0.5 Fe 2 O 4 is a reusability catalyst in activating PDS for CIP degradation.

研究领域: 环境科学 · 材料科学 · 化学工程
✓ 已验证 DOI 高影响因子
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Coating Porous TiO2 Films on Carbon Nanotubes to Enhance the Durability of Ultrafine PtCo/CNT Nanocatalysts for the Oxygen Reduction Reaction

Feng Cao,Hongyu Zhang,Xiao Duan,Xiaoke Li,Rui Ding,Kang Hua,Zhiyan Rui,Yongkang Wu,Mengchen Yuan,Jiankang Wang,Jia Li,Min Han,Jianguo Liu

The development of excellent activity and durability catalysts for the oxygen reduction reaction (ORR) is essential for the commercialization of proton exchange membrane fuel cells (PEMFCs). Reducing the size of catalyst particles can provide more reaction sites to mitigate the performance degradation caused by reduced platinum loading. However, at the same time, it makes the particles more prone to agglomeration and exfoliation, leading to a rapid reduction in catalyst activity. Here, we present the design of a composite support (TiO2/CNT) with a porous TiO2 film that immobilizes PtCo nanoparticles (NPs) loaded on the support while protecting the carbon nanotubes inside. The particle size of PtCo NPs was only 1.99 nm (determined by transmission electron microscopy), but the nanocatalyst (PtCo/TiO2/CNT) maintained high catalytic performance and stability on account of the strong metal support interaction (SMSI). PtCo/TiO2/CNT exhibited a high mass activity (MA, 0.476 A mgPt–1) and was found to have MA retention rates of 91.7 and 88.8% in durability tests performed at 0.6–1.0 V and 1.0–1.5 V, respectively.

研究领域: 材料科学 · 催化化学 · 燃料电池技术
✓ 已验证 DOI 高影响因子
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Applied Catalysis O: Open · 2024 · IF 0

Highly active palladium nanocatalyst for selective hydrogenation of 1,5-cyclooctadiene under atmospheric H2 pressure

Mingyang Liu,Yanhua Wang

An ionic liquid [CH 3 (OCH 2 CH 2 ) 22 N + Et 3 ][ p -CH 3 C 6 H 4 SO 3 − ] was synthesized and employed for stabilizing Pd nanocatalyst, which possesses the thermoregulated phase-separable property. The as-prepared Pd nanocatalyst was applied for the selective hydrogenation of 1,5-cyclooctadiene under atmospheric H 2 pressure. The >99% conversion of 1,5-cyclooctadiene with 95% selectivity towards cyclooctene was achieved under the optimal reaction conditions. The Pd nanocatalyst could be reused for six cycles without evident loss in conversion and selectivity. The turnover frequency of 4232 h −1 is greater than those of previously reported Pd nanocatalyst under atmospheric H 2 pressure.

研究领域: 催化化学 · 有机合成 · 纳米材料 · 绿色化学
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Scientific Reports · 2015 ·Vol. 5 ·期 1 ·1-8 · IF 5.578

Preparation of Hollow CuO@SiO2 Spheres and Its Catalytic Performances for the NO + CO and CO Oxidation

Niu Xiaoyu,Zhao Tieying,Yuan Fulong,Zhu Yujun

The hollow CuO@SiO 2 spheres with a mean diameter of 240 nm and a thin shell layer of about 30 nm in thickness was synthesized using an inorganic SiO 2 shell coating on the surface of Cu@C composite that was prepared by a two-step hydrothermal method. The obtained hollow CuO@SiO 2 spheres were characterized by ICP-AES, nitrogen adsorption-desorption, SEM, TEM, XRD, H 2 -TPR, CO-TPR, CO-TPD and NO-TPD. The results revealed that the hollow CuO@SiO 2 spheres consist of CuO uniformly inserted into SiO 2 layer. The CuO@SiO 2 sample exhibits particular catalytic activities for CO oxidation and NO + CO reactions compared with CuO supported on SiO 2 (CuO/SiO 2 ). The higher catalytic activity is attributed to the special hollow shell structure that possesses much more highly dispersed CuO nanocluster that can be easy toward the CO and NO adsorption and the oxidation of CO on its surface.

研究领域: 材料化学 · 催化化学 · 纳米材料科学 · 环境催化 · 无机合成
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Science China-Technological Sciences · 2022 ·Vol. 65 ·期 10 ·2317-2324 · IF 3.903

Oxygen-vacancy-rich TiO2 enables highly active and durable water electrolysis of urchin-like RuO2 catalyst

Gao HongMei,Xiao MeiLing,Li GuoQiang,Gao LiQin,Meng QingLei,Luo ZhaoYan,Luo ErGui,Liu ChangPeng,Jin Zhao,Ge JunJie,Xing Wei

The material innovation is prerequisite to accelerating sluggish oxygen evolution reaction (OER) kinetics, thus promoting the realization of hydrogen energy community. Herein, we develop an oxygen-vacancy-rich TiO 2 supported RuO 2 catalyst (RuO 2 @r-TiO 2 ) towards improved OER activity and stability. The oxygen vacancy on TiO 2 not only supplies electrons to produce lower valence Ru, but also provides sufficient anchoring site for the deposition of RuO 2 nanocrystal. Beyond that, it can generate strong electronic interaction between TiO 2 and supported RuO 2 , and thereby tailors the intermediates’ adsorption energy on the RuO 2 surface. As a result, the derived RuO 2 @r-TiO 2 catalyst exhibits superior OER activity and stability with the overpotential of 211 mV at a current density of 10 mA cm −2 and negligible activity degradation after 6 h operation, outperforming the non-oxygen-vacancy counterpart (223.3 mV, 12.75% activity loss) and RuO 2 catalyst (234.6 mV, 42.86% activity loss).

研究领域: 材料科学 · 电化学 · 催化化学 · 能源材料 · 纳米科技 · 物理化学
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ChemistrySelect · 2022 ·Vol. 7 ·期 45 ·e202204071 · IF 2.307

Synthesis of Ultrafine Platinum Nanocatalysts by Ice-photochemical Method and Their Application in Catalytic Degradation of 4-nitrophenol

Liang Xian,Jing Ma,Wei Li,Yanzhong Yang,Xu Gao,Bei Xi,Xiaoxia Tian

Graphical Under visible light irradiation at low temperature, uniformly dispersed ultrafine platinum(Pt) nanocatalysts was loaded on fullerene (C 60 ) without adding any reducing agent or stabilizing agent, and was effectively used to catalyze the reduction of 4-nitrophenol. The results show that Pt nanoparticles with good catalytic activity can be finally formed under the action of visible light. This green visible light chemical synthesis method is expected to be popularized in the field of catalysis. Here, uniformly dispersed ultrafine platinum nanocatalysts (Pt/C 60 ) were synthesized on C 60 by ice-photochemical method using potassium chloroplatinate (K 2 [PtCl 4 ]) as platinum source under the condition of low temperature, no stabilizer and reducing agent. X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS) and Transmission electron microscopy (TEM) were used to study the composition and morphology of Pt/C 60 catalyst. It was confirmed that Pt Ultra-small Particles (Pt UPs) was loaded on C 60 surface with high dispersion. The average particle sizes of the three samples obtained under different reaction conditions were 1.41±0.1 nm, 1.54±0.4 nm and 1.73±0.3 nm, respectively. The results show that the light-induced effect and the ice lattice domain limiting effect in the frozen state effectively control the formation and growth of platinum clusters in the process of Pt 2+ reduction to Pt 0 . The rate constants of the three samples were 0.89 min −1 , 0.31 min −1 , 0.19 min −1 , respectively, showing high catalytic activity in the study of the catalytic performance of Pt/C 60 degradation of 4-nitrophenol (4-NP) by Ultraviolet-visible spectroscopy (UV-Vis). This method provides a meaningful attempt for the study of green chemical synthesis method of platinum metal catalysts.

研究领域: 催化材料 · 环境科学 · 纳米技术
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2022 · IF 7.139

Metal-organic framework derived ellipse-like NiS2 nanocatalyst for stable electrochemical hydrogen generation in alkaline electrolyte

Shumin Wang,Yi Zhang,Xiaoyang Deng,Zizai Ma,Hefeng Yuan,Jinping Li,Xiaoguang Wang

The development of non-precious and high-efficient electrocatalysts to enhance the activity and stability in alkaline media is impending for massive hydrogen and oxygen production. In this study, NiS 2 nanoparticles array with ellipse-like topography was fabricated via simple hydrothermal and sulfurization treatment. The NiS 2 -400 featured with the unique loose stacking topographic architecture contributes to more exposed active sites, the smaller contact resistance between electrode/electrolyte, faster ion diffusion and electron transfer . As a result, NiS 2 -400 electrode requires only overpotentials of 116 and 178 mV to drive current densities of 10 and 50 mA cm −2 in 1.0 M KOH towards the hydrogen evolution reaction (HER), coupled with a Tafel slope of 93.0 mV dec −1 . Moreover, the resultant NiS 2 -400 nanoparticles exhibit excellent electrochemical stability for more than 50 h. In addition, the density functional theory (DFT) calculation further confirms that the (200) facet acts as the predominant active site, contributing to the enhanced HER performance.

研究领域: 材料科学 · 电化学
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