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>In situ growth of phosphorized ZIF-67-derived amorphous CoP/Cu2sub>O@CF electrocatalyst

《化学科学与工程前沿（英文）》 2023年第17卷第10期页码 1430-1439 doi: 10.1007/s11705-023-2320-1

摘要： Transition metal phosphides have been extensively studied for catalytic applications in water splitting. Herein, we report an in situ phosphorization of zeolitic imidazole frameworks (ZIF-67) to generate amorphous cobalt phosphide/ZIF-67 heterojunction on a self-supporting copper foam (CF) substrate with excellent performance for hydrogen evolution reaction (HER). The needle-leaf like copper hydroxide was anchored on CF surface, which acted as implantation to grow ZIF-67. The intermediate product was phosphorized to obtain final electrocatalyst (CoP/Cu₂O@CF) with uniform particle size, exhibiting a rhombic dodecahedron structure with wrinkles on the surface. The electrochemical measurement proved that CoP/Cu₂O@CF catalyst exhibited excellent HER activity and long-term stability in 1.0 mol·L^–1 KOH solution. The overpotential was only 62 mV with the Tafel slope of 83 mV·dec^–1 at a current density of 10 mA·cm^–2, with a large electrochemical active surface area. It also showed competitive performance at large current which indicated the potential application to industrial water electrolysis to produce hydrogen. First-principle calculations illustrated that benefit from the construction of CoP/ZIF-67 heterojunction, the d-band center of CoP downshifted after bonding with ZIF-67 and the Gibbs free energy (ΔG_H*) changed from –0.18 to –0.11 eV, confirming both decrease in overpotential and excellent HER activity. This work illustrates the efficient HER activity of CoP/Cu₂O@CF catalyst, which will act as a potential candidate for precious metal electrocatalysts.

关键词： CoP/Cu₂O@CF electrocatalyst phosphorization HER DFT

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Preparation of Cu/ZnO/Al

Hui FAN, Huayan ZHENG, Zhong LI

《化学科学与工程前沿（英文）》 2010年第4卷第4期页码 445-451 doi: 10.1007/s11705-010-0521-x

摘要： Cu/ZnO/Al O catalysts with Cu/Zn/Al ratios of 6/3/1 were precipitated and aged by conventional and microwave heating methods and tested in the slurry phase reactor for methanol synthesis. The effect of technological condition of precipitation and aging process under microwave irradiation on the catalytic performance was investigated to optimize the preparing condition of Cu/ZnO/Al O catalyst. The results showed that the microwave irradiation during precipitation process could improve the activity of the catalyst, but had little effect on the stability. While the microwave irradiation during aging process has a great benefit to both the activity and stability of the catalyst, the catalyst aged at 80°C for 1 h under microwave irradiation possessed higher methanol space time yield (STY) and more stable catalytic activity. The activity and stability of the catalyst was further enhanced when microwave irradiation was used in both precipitation and aging processes; the optimized condition for the catalyst precursor preparation was precipitation at 60°C and aging at 80°C under microwave irradiation.

关键词： microwave irradiation precipitation temperature aging temperature methanol synthesis Cu/ZnO/Al₂O₃ catalyst

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Catalytic hydrolysis of gaseous HCN over Cu–Ni/γ-Al

Linxia Yan, Senlin Tian, Jian Zhou, Xin Yuan

《环境科学与工程前沿（英文）》 2016年第10卷第6期 doi: 10.1007/s11783-016-0872-8

摘要： ? The Cu–Ni/γ-Al O catalyst was prepared to study HCN hydrolysis ? On catalyst calcined at 400°C, the HCN removal efficiency reaches a maximum. ? HCN removal is the highest at 480 min at a H O/HCN volume ratio of 150 ? The presence of CO facilitates HCN hydrolysis and increases NH production. ? O increases the HCN removal and NO production but decreases NH production GRAPHIC ABSTRACT To decompose efficiently hydrogen cyanide (HCN) in exhaust gas, g-Al O -supported bimetallic-based Cu–Ni catalyst was prepared by incipient-wetness impregnation method. The effects of the calcination temperature, H O/HCN volume ratio, reaction temperature, and the presence of CO or O on the HCN removal efficiency on the Cu–Ni/g-Al O catalyst were investigated. To examine further the efficiency of HCN hydrolysis, degradation products were analyzed. The results indicate that the HCN removal efficiency increases and then decreases with increasing calcination temperature and H O/HCN volume ratio. On catalyst calcined at 400°C, the efficiency reaches a maximum close to 99% at 480 min at a H O/HCN volume ratio of 150. The HCN removal efficiency increases with increasing reaction temperature within the range of 100°C–500°C and reaches a maximum at 500°C. This trend may be attributed to the endothermicity of HCN hydrolysis; increasing the temperature favors HCN hydrolysis. However, the removal efficiencies increases very few at 500°C compared with that at 400°C. To conserve energy in industrial operations, 400°C is deemed as the optimal reaction temperature. The presence of CO facilitates HCN hydrolysis andincreases NH production. O substantially increases the HCN removal efficiency and NO production but decreases NH production.

关键词： Hydrogen cyanide Cu–Ni/g-Al₂O₃ Catalytic hydrolysis

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Rh2sub>O3sub>/hexagonal CePO4sub> nanocatalysts for N2sub>O decomposition

Huan Liu, Zhen Ma

《化学科学与工程前沿（英文）》 2017年第11卷第4期页码 586-593 doi: 10.1007/s11705-017-1659-6

摘要： Hexagonal CePO nanorods were prepared by a precipitation method and hexagonal CePO nanowires were prepared by hydrothermal synthesis at 150 °C. Rh(NO ) was then used as a precursor for the impregnation of Rh O onto these CePO materials. The Rh O supported on the CePO nanowires was much more active for the catalytic decomposition of N O than the Rh O supported on CePO nanorods. The stability of both catalysts as a function of time on stream was studied and the influence of the co-feed (CO , O , H O or O /H O) on the N O decomposition was also investigated. The samples were characterized by N adsorption-desorption, inductively coupled plasma optical emission spectroscopy, X-ray diffraction, transmission electron microscopy, X-ray photoelectron microscopy, hydrogen temperature-programmed reduction, oxygen temperature-programmed desorption, and CO temperature-programmed desorption in order to correlate the physicochemical and catalytic properties.

关键词： Rh₂O₃ CePO₄ N₂O decomposition

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Preparation of Cu/ZrO

Xinmei LIU, Shaofen BAI, Huidong ZHUANG, Zifeng YAN

《化学科学与工程前沿（英文）》 2012年第6卷第1期页码 47-52 doi: 10.1007/s11705-011-1170-4

摘要： Cu/ZrO catalysts for methanol synthesis from CO /H were respectively prepared by deposition coprecipitation (DP) and solid state reaction (SR) methods. There is an intimate interaction between copper and zirconia, which strongly affects the reduction property and catalytic performance of the catalysts. The stronger the interaction, the lower the reduction temperature and the better the performance of the catalysts. Surface area, pore structure and crystal structure of the catalysts are mainly controlled by preparation methods and alkalinity of synthesis system. The conversion of CO and selectivity of methanol are higher for DP catalysts than for SP catalysts.

关键词： Cu/ZrO₂ methanol synthesis deposition coprecipitation solid state reaction CO₂/H₂

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Cu-doped Bi/Bi2sub>WO6sub> catalysts for efficient N2sub> fixation by photocatalysis

《化学科学与工程前沿（英文）》 2023年第17卷第10期页码 1412-1422 doi: 10.1007/s11705-023-2312-1

摘要： In this paper, Cu-doped Bi₂WO₆ was synthesized via a solvothermal method and applied it in photocatalytic N₂ immobilization. Characterization results showed the presence of a small amount of metallic Bi in the photocatalyst, indicating that the synthesized photocatalyst is actually Bi/Cu-Bi₂WO₆ composite. The doped Cu had a valence state of +2 and most likely substituted the position of Bi³⁺. The introduced Cu did not affect the metallic Bi content, but mainly influenced the energy band structure of Bi₂WO₆. The band gap was slightly narrowed, the conduction band was elevated, and the work function was reduced. The reduced work function improved the transfer and separation of charge carriers, which mainly caused the increased photoactivity. The optimized NH₃ generation rates of Bi/Cu-Bi₂WO₆ reached 624 and 243 μmol·L^–1·g^–1·h^–1 under simulated solar and visible light, and these values were approximately 2.8 and 5.9 times higher those of Bi/Bi₂WO₆, respectively. This research provides a method for improving the photocatalytic N₂ fixation and may provide more information on the design and preparation of heteroatom-doped semiconductor photocatalysts for N₂-to-NH₃ conversion.

关键词： Bi₂WO₆ Cu doping work function photocatalytic N₂ fixation charge separation

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The stabilization effect of Al2sub>O3sub> on unconventional Pb/SiO2sub> catalyst

《化学科学与工程前沿（英文）》 2023年第17卷第10期页码 1423-1429 doi: 10.1007/s11705-023-2315-y

摘要： Similar to Sn, Pb located at the same group (IVA) in the periodic table of elements, can also catalyze propane dehydrogenation to propene, while a fast deactivation can be observed. To enhance the stability, the traditional carrier Al₂O₃ with a small amount, was introduced into Pb/SiO₂ catalyst in this study. It has been proved that Al₂O₃ can inhibit the reduction of PbO, and weaken the agglomeration and loss of Pb species due to its enhanced interaction with Pb species. As a result, 3Al15Pb/SiO₂ catalyst exhibits a much higher stability up to more than 150 h. In addition, a simple schematic diagram of the change of surface species on the catalyst surface after Al₂O₃ addition was also proposed.

关键词： Pb/SiO₂ Al₂O₃ propane dehydrogenation propene stability

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固体氧化物电解池共电解H2sub>O/CO2sub>研究进展

范慧,宋世栋,韩敏芳

《中国工程科学》 2013年第15卷第2期页码 107-112

摘要：本文介绍了固体氧化物电解池的结构特点及其用于H2O/CO2的共电解制备H2和CO的工作原理，综述了固体氧化物电解池的组成形式，以及单片电解池和电解池堆用于H2O/CO2共电解反应的国内外研究进展，并阐述了提高固体氧化物电解池共电解效率所亟需解决的问题

关键词：固体氧化物电解池 H2sub>O/CO2sub>共电解合成气电解效率水电解

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含稀释剂的Al-Cr2sub>O3sub>体系燃烧合成反应热力学分析与反应模型

张衍诚,潘冶,张传

《中国工程科学》 2004年第6卷第6期页码 63-67

摘要：

对含稀释剂Al203和Cr203的Al-Cr203体系燃烧合成反应进行了热力学计算与分析，讨论了起始反应温度T0、稀释剂Al2O3和Cr2O3的含量对绝热反应温度7^的影响，并得出T0与Tad在特定温度段上的近似线性关系以及该关系在指导材料成分设计上的应用；揭示了反应驱动力—&mdash

关键词：金属陶瓷燃烧合成 Al-Cr203体系热力学反应模型

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ZnFe2sub>O4sub> deposited on BiOCl with exposed (001) and (010) facets for photocatalyticreduction of CO2sub> in cyclohexanol

Guixian Song, Xionggang Wu, Feng Xin, Xiaohong Yin

《化学科学与工程前沿（英文）》 2017年第11卷第2期页码 197-204 doi: 10.1007/s11705-016-1606-y

摘要： ZnFe O -BiOCl composites were prepared by both hydrothermal and direct precipitation processes and the structures and properties of the samples were characterized by various instrumental techniques. The samples were then used as catalysts for the photocatalytic reduction of CO in cyclohexanol under ultraviolet irradiation to give cyclohexanone (CH) and cyclohexyl formate (CF). The photocatalytic CO reduction activities over the hydrothermally prepared ZnFe O -BiOCl composites were higher than those over the directly-precipitated composites. This is because compared to the direct-precipitation sample, the ZnFe O nanoparticles in the hydrothermal sample were smaller and more uniformly distributed on the surface of BiOCl and so more heterojunctions were formed. Higher CF and CH yields were obtained for the pure BiOCl and BiOCl composite samples with more exposed (001) facets than for the samples with more exposed (010) facets. This is due to the higher density of oxygen atoms in the exposed (001) facets, which creates more oxygen vacancies, and thereby improves the separation efficiency of the electron-hole pairs. More importantly, irradiation of the (001) facets with ultraviolet light produces photo-generated electrons which is helpful for the reduction of CO to ·CO . The mechanism for the photocatalytic reduction of CO in cyclohexanol over ZnFe O -BiOCl composites with exposed (001) facets involves electron transfer and carbon radical formation.

关键词： reduction of CO₂ cyclohexanol ZnFe₂O₄ deposited BiOCl facet composite photocatalyst

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Al2sub>O3sub>-Mxsub>Oysub>硬面陶瓷涂层的喷焊制备及性能研究

王飚,王宇栋,李慧玲,张自华

《中国工程科学》 2002年第4卷第9期页码 75-80

摘要：

在碳钢母材上，用氧乙炔焰喷焊镍包铝合金粉末制取预涂层，喷焊50% Al2sub>O3sub>+50% Ni的复合粉末制取过渡层，用等离子喷焊Al2sub>O3sub> - Mxsub>Oysub>复合粉末制取最终涂层。

关键词： Al2sub>O3sub>-Mxsub>Oysub> 涂层等离子抗腐蚀抗磨损

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Al2sub>O3sub> and CeO2sub>-promoted MgO sorbents for CO2sub> capture at moderate

Huimei Yu, Xiaoxing Wang, Zhu Shu, Mamoru Fujii, Chunshan Song

《化学科学与工程前沿（英文）》 2018年第12卷第1期页码 83-93 doi: 10.1007/s11705-017-1691-6

摘要： A series of Al O and CeO modified MgO sorbents was prepared and studied for CO sorption at moderate temperatures. The CO sorption capacity of MgO was enhanced with the addition of either Al O or CeO . Over Al O -MgO sorbents, the best capacity of 24.6 mg-CO /g-sorbent was attained at 100 °C, which was 61% higher than that of MgO (15.3 mg-CO /g-sorbent). The highest capacity of 35.3 mg-CO /g-sorbent was obtained over the CeO -MgO sorbents at the optimal temperature of 200 °C. Combining with the characterization results, we conclude that the promotion effect on CO sorption with the addition of Al O and CeO can be attributed to the increased surface area with reduced MgO crystallite size. Moreover, the addition of CeO increased the basicity of MgO phase, resulting in more increase in the CO capacity than Al O promoter. Both the Al O -MgO and CeO -MgO sorbents exhibited better cyclic stability than MgO over the course of fifteen CO sorption-desorption cycles. Compared to Al O , CeO is more effective for promoting the CO capacity of MgO. To enhance the CO capacity of MgO sorbent, increasing the basicity is more effective than the increase in the surface area.

关键词： CO₂ capture MgO sorbents Al₂O₃ CeO₂ flue gas

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CO2sub> methanation and co-methanation of CO and CO2sub> over Mn-promoted Ni/Al2sub>O3sub> catalysts

Kechao Zhao,Zhenhua Li,Li Bian

《化学科学与工程前沿（英文）》 2016年第10卷第2期页码 273-280 doi: 10.1007/s11705-016-1563-5

摘要： A series of Mn-promoted 15 wt-% Ni/Al O catalysts were prepared by an incipient wetness impregnation method. The effect of the Mn content on the activity of the Ni/Al O catalysts for CO methanation and the co-methanation of CO and CO in a fixed-bed reactor was investigated. The catalysts were characterized by N physisorption, hydrogen temperature-programmed reduction and desorption, carbon dioxide temperature-programmed desorption, X-ray diffraction and high-resolution transmission electron microscopy. The presence of Mn increased the number of CO adsorption sites and inhibited Ni particle agglomeration due to improved Ni dispersion and weakened interactions between the nickel species and the support. The Mn-promoted 15 wt-% Ni/Al O catalysts had improved CO methanation activity especially at low temperatures (250 to 400 °C). The Mn content was varied from 0.86% to 2.54% and the best CO conversion was achieved with the 1.71Mn-Ni/Al O catalyst. The co-methanation tests on the 1.71Mn-Ni/Al O catalyst indicated that adding Mn markedly enhanced the CO methanation activity especially at low temperatures but it had little influence on the CO methanation performance. CO methanation was more sensitive to the reaction temperature and the space velocity than the CO methanation in the co-methanation process.

关键词： Mn promotion nickel catalysts CO₂ methanation co-methanation of CO and CO₂

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ZnFe2sub>O4sub>/BiVO4sub> Z-scheme heterojunction for efficient visible-light photocatalytic

《化学科学与工程前沿（英文）》 2023年第17卷第11期页码 1728-1740 doi: 10.1007/s11705-023-2322-z

摘要： A novel Z-scheme ZnFe₂O₄/BiVO₄ heterojunction photocatalyst was successfully synthesized using a convenient solvothermal method and applied in the visible light photocatalytic degradation of ciprofloxacin, which is a typical antibiotic contaminant in wastewater. The heterostructure of as-synthesized catalysts was confirmed using X-ray diffraction, scanning electron microscopy, transmission electron microscopy and X-ray photoelectron spectroscopy characterizations. Compared with the single-phase counterparts, ZnFe₂O₄/BiVO₄ demonstrated considerably enhanced photogenerated charge separation efficiencies because of the Z-scheme transfer mechanism of electrons between the composite photocatalysts. Consequently, the 30% ZnFe₂O₄/BiVO₄ catalyst afforded a degradation rate of up to 97% of 20 mg/L ciprofloxacin under 30 min of visible light irradiation with a total organic carbon removal rate of 50%, which is an excellent activity compared with ever reported BiVO₄-based catalysts. In addition, the liquid chromatography-mass spectrometry and quantitative structure-activity relationships model analyses demonstrated that the toxicity of the intermediates was lower than that of the parent ciprofloxacin. Moreover, the as-synthesized ZnFe₂O₄/BiVO₄ heterojunctions were quite stable and could be reused at least four times. This study thus provides a promising Z-scheme heterojunction photocatalyst for the efficient removal and detoxication of antibiotic pollutants from wastewater.

关键词： ZnFe₂O₄/BiVO₄ Z-scheme heterojunction photocatalytic degradation ciprofloxacin