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催化剂 2

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Pt–Ba–Ce/γ-Al2O3 催化剂，物理化学性质，NOx存储和还原，NOx 排放，H2 还原剂 1

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Enhanced activity of bimetallic Fe-Cu catalysts supported on ceria toward water gas shift reaction: synergistic

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 1962-1972 doi: 10.1007/s11705-023-2359-z

摘要： Within the “hydrogen chain”, the high-temperature water gas shift reaction represents a key step to improve the H2 yield and adjust the H2/COx ratio to fit the constraints of downstream processes. Despite the commercial application of the high-temperature water gas shift, novel catalysts characterized by higher intrinsic activity (especially at low temperatures), good thermal stability, and no chromium content are needed. In this work, we propose bimetallic iron-copper catalysts supported on ceria, characterized by low active phase content (iron oxide + copper oxide < 5 wt %). Fresh and used samples were characterized by inductively coupled plasma mass spectrometry, X-ray diffraction, nitrogen physisorption, scanning electron microscopy coupled with energy-dispersive X-ray spectroscopy, and temperature programmed reduction in hydrogen to relate physicochemical features and catalytic activity. The sample with iron/copper ≈ 1 and 4 wt % active phase content showed the best catalytic properties in terms of turnover frequency, no methane formation, and stability. Its unique properties were due to both strong iron-copper interaction and strong metal-support interaction, leading to outstanding redox behavior.

关键词： water gas shift     iron     copper     bimetallic catalysts     ceria     hydrogen    

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The synergic effects of highly selective bimetallic Pt-Pd/SAPO-41 catalysts for the

Guozhi Jia, Chunmu Guo, Wei Wang, Xuefeng Bai, Xiaomeng Wei, Xiaofang Su, Tong Li, Linfei Xiao, Wei Wu

《化学科学与工程前沿（英文）》 2021年 第15卷 第5期   页码 1111-1124 doi: 10.1007/s11705-020-2031-9

摘要： The hydroisomerization of -hexadecane over Pt-Pd bimetallic catalysts is an effective way to produce clean fuel oil. This work reports a useful preparation method of bimetallic bifunctional catalysts by a co-impregnation or sequential impregnation process. Furthermore, monometallic catalysts with loading either Pt or Pd are also prepared for comparison. The effects of the metal species and impregnation order on the characteristics and catalytic performance of the catalysts are investigated. The catalytic test results indicate that the maximum -hexadecane yield over different catalysts increases as follows: Pt/silicoaluminophosphate SAPO-41

关键词： SAPO-41 molecular sieve     Pt-Pd bimetallic site     bifunctional catalysts     n-hexadecane     hydroisomerization    

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Bimetallic Ni-Fe catalysts derived from layered double hydroxides for CO methanation from syngas

Honggui Tang, Shuangshuang Li, Dandan Gong, Yi Guan, Yuan Liu

《化学科学与工程前沿（英文）》 2017年 第11卷 第4期   页码 613-623 doi: 10.1007/s11705-017-1664-9

摘要： Carbon deposition and sintering of active components such as nano particles are great challenges for Ni-based catalysts for CO methanation to generate synthetic natural gas from syngas. Facing the challenges, bimetallic catalysts with different Fe content derived from layered double hydroxide containing Ni, Fe, Mg, Al elements were prepared by co-precipitation method. Nanoparticles of Ni-Fe alloy were supported on mixed oxides of aluminium and magnesium after calcination and reduction. The catalysts were characterized by Brunner-Emmett-Teller (BET), X-ray diffraction, hydrogen temperature programmed reduction, inductively coupled plasma, X-ray photoelectron spectroscopy, transmission electron microscopy and thermogravimetric techniques, and their catalytic activity for CO methanation was investigated. The results show that the Ni-Fe alloy catalysts exhibit better catalytic performance than monometallic catalysts except for the Ni4Fe-red catalyst. The Ni2Fe-red catalyst shows the highest CO conversion (100% at 260–350 °C), as well as the highest CH selectivity (over 95% at 280–350 °C), owing to the formation of Ni-Fe alloy. In stability test, the Ni2Fe-red catalyst exhibits great improvement in both anti-sintering and resistance to carbon formation compared with the Ni0Fe-red catalyst. The strong interaction between Ni and Fe element in alloy and surface distribution of Fe element not only inhibits the sintering of nanoparticles but restrains the formation of Ni clusters.

关键词： methanation     layered double hydroxide     bimetal Ni-Fe alloy     sintering     carbon deposition    

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Pd-Ni nanoparticles supported on titanium oxide as effective catalysts for Suzuki-Miyaura coupling reactions

Dongxu Han, Zhiguo Zhang, Zongbi Bao, Huabin Xing, Qilong Ren

《化学科学与工程前沿（英文）》 2018年 第12卷 第1期   页码 24-31 doi: 10.1007/s11705-017-1669-4

摘要： We have successfully prepared a series of Pd-Ni/TiO catalysts by a one-step impregnation-reduction method. Among these catalysts with different compositions of Ni and Pd, the one with the Ni:Pd ratio of 2.95 showed the best activity. Small monodispersed Pd-Ni bimetallic nanoparticles were loaded on the surface of titanium oxide nanopowder as confirmed with TEM and EDS mapping. The XPS analysis demonstrated that Pd exists as 31% Pd(II) species and 69% Pd(0) species and all nickel is Ni(II). The prepared Pd-Ni/TiO exhibited enhanced catalytic activity compared to an equal amount of Pd/TiO for Suzuki-Miyaura reactions together with excellent applicability and reusability.

关键词： Pd-Ni bimetallic nanoparticles     nanocatalysis     Suzuki-Miyaura reaction     titanium oxide    

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Investigation of the preparation methodologies of Pd-Cu single atom alloy catalysts for selective hydrogenation

Xinxiang Cao,Arash Mirjalili,James Wheeler,Wentao Xie,Ben W.-L. Jang

《化学科学与工程前沿（英文）》 2015年 第9卷 第4期   页码 442-449 doi: 10.1007/s11705-015-1547-x

摘要： Galvanic replacement, co-impregnation and sequential impregnation have been employed to prepare Pd-Cu bimetallic catalysts with less than 1 wt-% Cu and ca. 0.03 wt-% Pd for selective hydrogenation of acetylene in excess ethylene. High angle annular dark field-scanning transmission electron microscopy (HAADF-STEM) and H chemisorption results confirmed that Pd-Cu single-atom alloy structures were constructed in all three bimetallic catalysts. Catalytic tests indicated that when the conversion of acetylene was above 99%, the selectivity of ethylene of these three single atom alloy catalysts was still more than 73%. Furthermore, the single atom alloy catalyst prepared by sequential incipient wetness impregnation was found to have the best stability among the three procedures used.

关键词： H2 pulse chemisorption     palladium-copper bimetallic catalyst     single atom alloy     acetylene hydrogenation     HAADF-STEM    

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Ni-Co bimetallic catalyst for CH

Xiaohong LI, Jun AI, Wenying LI, Dongxiong LI

《化学科学与工程前沿（英文）》 2010年 第4卷 第4期   页码 476-480 doi: 10.1007/s11705-010-0512-y

摘要： A co-precipitation method was employed to prepare Ni/Al O -ZrO , Co/Al O -ZrO and Ni-Co/Al O -ZrO catalysts. Their properties were characterized by N adsorption (BET), thermogravimetric analysis TGA , temperature-programmed reduction (TPR), temperature-programmed desorption (CO -TPD), and temperature-programmed surface reaction (CH -TPSR and CO -TPSR). Ni-Co/Al O -ZrO bimetallic catalyst has good performance in the reduction of active components Ni, Co and CO adsorption. Compared with mono-metallic catalyst, bimetallic catalyst could provide more active sites and CO adsorption sites (C+ CO = 2CO) for the methane-reforming reaction, and a more appropriate force formed between active components and composite support (SMSI) for the catalytic reaction. According to the CH -CO -TPSR, there were 80.9% and 81.5% higher CH and CO conversion over Ni-Co/Al O -ZrO catalyst, and its better resistance to carbon deposition, less than 0.5% of coke after 4 h reaction, was found by TGA. The high activity and excellent anti-coking of the Ni-Co/Al O -ZrO catalyst were closely related to the synergy between Ni and Co active metal, the strong metal-support interaction and the use of composite support.

关键词： Ni-Co bimetallic catalyst     composite support     CH4 reforming with CO2    

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Enhanced activation of persulfate using mesoporous silica spheres augmented Cu–Al bimetallic oxide particles

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1581-1592 doi: 10.1007/s11705-023-2327-7

摘要： Herein, Cu–Al bimetallic oxide was synthesized and mixed with mesoporous silica spheres via a simple hydrothermal method. The prepared sample was then analyzed and employed to activate potassium peroxydisulfate for bisphenol A removal. Based on the results of X-ray diffraction, scanning electron microscopy, and energy dispersion spectroscopy, Cu–Al bimetallic oxide was determined as CuO-Al2O3, and mesoporous silica spheres were found around the these particles. At 30 min, a bisphenol A degradation level of 90% was achieved, and it remained at over 60% after five consecutive cycles, indicating the catalyst’s superior capacity and stability. In terms of removal performance, the radical pathway (including SO4•‒, OH •, and O2•‒) and singlet oxygen (1O2) played minor roles, while electron migration between bisphenol A, potassium peroxydisulfate, and the catalyst played a dominant role. The introduction of Al2O3 promoted the formation of surface oxygen vacancies, which improved ligand complex formation between potassium peroxydisulfate and the catalyst, thereby facilitating electron migration. Furthermore, mesoporous silica spheres augment not only enhanced bisphenol A adsorption but also alleviated Cu leaching. Overall, this work is expected to provide significant support for the rational development of catalysts with high catalytic activity for persulfate activation via surface electron migration.

关键词： Cu–Al bimetallic oxides     mesoporous silica spheres     peroxydisulfate     bisphenol A    

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Fabrication of bimetallic Cu–Zn adsorbents with high dispersion by using confined space for gas adsorptive

《化学科学与工程前沿（英文）》   页码 1623-1631 doi: 10.1007/s11705-022-2202-y

摘要： The number of active components and their dispersion degree are two key factors affecting the performance of adsorbents. Here, we report a simple but efficient strategy for dispersing active components by using a confined space, which is formed by mesoporous silica walls and templates in the as-prepared SBA-15 (AS). Such a confined space does not exist in the conventional support, calcined SBA-15, which does not contain a template. The Cu and Zn precursors were introduced to the confined space in the AS and were converted to CuO and ZnO during calcination, during which the template was also removed. The results show that up to 5 mmol·g–1 of CuO and ZnO can be well dispersed; however, severe aggregation of both oxides takes place in the sample derived from the calcined SBA-15 with the same loading. Confined space in the AS and the strong interactions caused by the abundant hydroxyl groups are responsible for the dispersion of CuO and ZnO. The bimetallic materials were employed for the adsorptive separation of propene and propane. The samples prepared from the as-prepared SBA-15 showed superior performance to their counterparts from the calcined SBA-15 in terms of both adsorption capacity of propene and selectivity for propene/propane.

关键词： bimetallic adsorbents     confined space     mesoporous silica     propene/propane separation    

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Removing polybrominated diphenyl ethers in pure water using Fe/Pd bimetallic nanoparticles

Min ZHANG,Jian LU,Zhencheng XU,Yiliang HE,Bo ZHANG,Song JIN,Brian BOMAN

《环境科学与工程前沿（英文）》 2015年 第9卷 第5期   页码 832-839 doi: 10.1007/s11783-015-0778-x

摘要： Polybrominated diphenyl ethers (PBDEs) have been widely used as fire-retardants. Due to their high production volume, widespread usage, and environmental persistence, PBDEs have become ubiquitous contaminants in various environments.Nanoscale zero-valent iron (ZVI) is an effective reductant for many halogenated organic compounds. To enhance the degradation efficiency, ZVI/Palladium bimetallic nanoparticles (nZVI/Pd) were synthesized in this study to degrade decabromodiphenyl ether (BDE209) in water. Approximately 90% of BDE209 was rapidly removed by nZVI/Pd within 80 min, whereas about 25% of BDE209 was removed by nZVI. Degradation of BDE209 by nZVI/Pd fits pseudo-first-order kinetics. An increase in pH led to sharply decrease the rate of BDE209 degradation. The degradation rate constant in the treatment with initial pH at 9.0 was more than 6.8 × higher than that under pH 5.0. The degradation intermediates of BDE209 by nZVI/Pd were identified and the degradation pathways were hypothesized. Results from this study suggest that nZVI/Pd may be an effective tool for treating polybrominated diphenyl ethers (PBDEs) in water.

关键词： degradation     bimetallic nanoparticles     nanoscale zero-valent iron     polybrominated diphenyl ethers    

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Dechlorination of dichlorodiphenyltrichloroethane (DDT) by Fe/Pd bimetallic nanoparticles: Comparison

Kubra Ulucan-Altuntas, Eyup Debik

《环境科学与工程前沿（英文）》 2020年 第14卷 第1期 doi: 10.1007/s11783-019-1196-2

摘要： DDT undergoes dechlorination via Fe/Pd bimetallic nanoparticle. The oxidation effect of nZVI on DDT is greatly improved when Pd is dopped. The highest concentration to be treated under cancerogenesis limit was 110 mg/L. The dechlorination of DDT is more like to DDE via Fe/Pd but to DDD via nZVI. Degradation products concentrations are lowered via Fe/Pd when compared with nZVI. In this study, the bimetallic Fe/Pd nanoparticle was synthesized using the catalytic element palladium to increase the effect of nano zero valent iron (nZVI), in the light of the information obtained from our previous study, in which the nZVI synthesis method was modified. Dichlorodiphenyltrichloroethane (DDT), one of the most widely used persistent organic pollutant pesticides in the world, was investigated in terms of its degradation by Fe/Pd nanoparticles and the difference with nZVI was determined. During the study, the Fe/Pd concentration, initial DDT concentration, and contact time were selected as variables affecting the treatment. The highest possible initial DDT concentration for the treatment with Fe/Pd bimetallic nanoparticle was investigated to obtain the DDT effluent concentration below the carcinogenesis limit, 0.23 µg/L. The highest concentration that could be treated was found to be 109.95 mg/L with Fe/Pd. It was found that 44.3 min of contact time and 550 mg/L Fe/Pd concentration were needed to achieve this treatment.

关键词： Persistent organic pollutants     nZVI     Bimetallic nanoparticle     Organochlorine pesticides     DDT    

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Mechanistic understanding of Cu-based bimetallic catalysts

You Han, Yulian Wang, Tengzhou Ma, Wei Li, Jinli Zhang, Minhua Zhang

《化学科学与工程前沿（英文）》 2020年 第14卷 第5期   页码 689-748 doi: 10.1007/s11705-019-1902-4

摘要： Copper has received extensive attention in the field of catalysis due to its rich natural reserves, low cost, and superior catalytic performance. Herein, we reviewed two modification mechanisms of co-catalyst on the coordination environment change of Cu-based catalysts: (1) change the electronic orbitals and geometric structure of Cu without any catalytic functions; (2) act as an additional active site with a certain catalytic function, as well as their catalytic mechanism in major reactions, including the hydrogenation to alcohols, dehydrogenation of alcohols, water gas shift reaction, reduction of nitrogenous compounds, electrocatalysis and others. The influencing mechanisms of different types of auxiliary metals on the structure-activity relationship of Cu-based catalysts in these reactions were especially summarized and discussed. The mechanistic understanding can provide significant guidance for the design and controllable synthesis of novel Cu-based catalysts used in many industrial reactions.

关键词： copper     bimetallic catalyst     coordination     modification mechanism     catalytic application    

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A Pt-Bi bimetallic nanoparticle catalyst for direct electro-oxidation of formic acid in fuel cells

Shu-Hong LI, Yue ZHAO, Jian CHU, Wen-Wei LI, Han-Qing YU, Gang LIU, Yang-Chao TIAN

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 388-394 doi: 10.1007/s11783-012-0475-y

摘要： Direct formic acid fuel cells are a promising portable power-generating device, and the development of efficient anodic catalysts is essential for such a fuel cell. In this work Pt-Bi nanoparticles supported on micro-fabricated gold wire array substrate were synthesized using an electrochemical deposition method for formic acid oxidation in fuel cells. The surface morphology and element components of the Pt-Bi/Au nanoparticles were characterized, and the catalytic activities of the three Pt-Bi/Au nanoparticle electrodes with different Pt/Bi ratios for formic acid oxidation were evaluated. It was found that Pt Bi /Au had a much higher catalytic activity than Pt Bi /Au and Pt Bi /Au, and Pt Bi /Au exhibited a current density of 2.7 mA·cm , which was 27-times greater than that of Pt/Au. The electro-catalytic activity of the Pt-Bi/Au electrode for formic acid oxidation increased with the increasing Bi content, suggesting that it would be possible to achieve an efficient formic acid oxidation on the low Pt-loading. Therefore, the Pt-Bi/Au electrode offers a promising catalyst with a high activity for direct oxidation of formic acid in fuel cells.

关键词： catalyst     electrochemical deposition     formic acid oxidation     fuel cell     gold wire array     microfabrication    

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Electrochemical CO reduction to C products over CuZn intermetallic catalysts synthesized by electrodeposition

《能源前沿（英文）》 doi: 10.1007/s11708-023-0898-0

摘要： Electrocatalytic CO2 reduction (ECR) offers an attractive approach to realizing carbon neutrality and producing valuable chemicals and fuels using CO2 as the feedstock. However, the lack of cost-effective electrocatalysts with better performances has seriously hindered its application. Herein, a one-step co-electrodeposition method was used to introduce Zn, a metal with weak *CO binding energy, into Cu to form Cu/Zn intermetallic catalysts (Cu/Zn IMCs). It was shown that, using an H-cell, the high Faradaic efficiency of C2+ hydrocarbons/alcohols (FEC2+) could be achieved in ECR by adjusting the surface metal components and the applied potential. In suitable conditions, FEC2+ and current density could be as high as 75% and 40 mA/cm2, respectively. Compared with the Cu catalyst, the Cu/Zn IMCs have a lower interfacial charge transfer resistance and a larger electrochemically active surface area (ECSA), which accelerate the reaction. Moreover, the *CO formed on Zn sites can move to Cu sites due to its weak binding with *CO, and thus enhance the C–C coupling on the Cu surface to form C2+ products.

关键词： carbon dioxide electroreduction     electrochemistry     co-electrodeposition     intermetallic catalysts     value-added chemicals    

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Oxygen reduction electrocatalysis: From conventional to single-atomic platinum-based catalysts for proton

《能源前沿（英文）》 doi: 10.1007/s11708-023-0907-3

摘要： Platinum (Pt)-based materials are still the most efficient and practical catalysts to drive the sluggish kinetics of cathodic oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs). However, their catalysis and stability performance still need to be further improved in terms of corrosion of both carbon support and Pt catalyst particles as well as Pt loading reduction. Based on the developed synthetic strategies of alloying/nanostructuring Pt particles and modifying/innovating supports in developing conventional Pt-based catalysts, Pt single-atom catalysts (Pt SACs) as the recently burgeoning hot materials with a potential to achieve the maximum utilization of Pt are comprehensively reviewed in this paper. The design thoughts and synthesis of various isolated, alloyed, and nanoparticle-contained Pt SACs are summarized. The single-atomic Pt coordinating with non-metals and alloying with metals as well as the metal-support interactions of Pt single-atoms with carbon/non-carbon supports are emphasized in terms of the ORR activity and stability of the catalysts. To advance further research and development of Pt SACs for viable implementation in PEMFCs, various technical challenges and several potential research directions are outlined.

关键词： oxygen reduction electrocatalysis     Pt single-atom catalysts     conventional Pt-based catalysts     design thoughts and synthesis     metal-support interactions    

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Promising approach for preparing metallic single-atom catalysts: electrochemical deposition

《能源前沿（英文）》 2022年 第16卷 第4期   页码 537-541 doi: 10.1007/s11708-022-0837-5

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标题 作者 时间 类型 操作

Enhanced activity of bimetallic Fe-Cu catalysts supported on ceria toward water gas shift reaction: synergistic

期刊论文

The synergic effects of highly selective bimetallic Pt-Pd/SAPO-41 catalysts for the

Guozhi Jia, Chunmu Guo, Wei Wang, Xuefeng Bai, Xiaomeng Wei, Xiaofang Su, Tong Li, Linfei Xiao, Wei Wu

期刊论文

Bimetallic Ni-Fe catalysts derived from layered double hydroxides for CO methanation from syngas

Honggui Tang, Shuangshuang Li, Dandan Gong, Yi Guan, Yuan Liu

期刊论文

Pd-Ni nanoparticles supported on titanium oxide as effective catalysts for Suzuki-Miyaura coupling reactions

Dongxu Han, Zhiguo Zhang, Zongbi Bao, Huabin Xing, Qilong Ren

期刊论文

Investigation of the preparation methodologies of Pd-Cu single atom alloy catalysts for selective hydrogenation

Xinxiang Cao,Arash Mirjalili,James Wheeler,Wentao Xie,Ben W.-L. Jang

期刊论文

Ni-Co bimetallic catalyst for CH

Xiaohong LI, Jun AI, Wenying LI, Dongxiong LI

期刊论文

Enhanced activation of persulfate using mesoporous silica spheres augmented Cu–Al bimetallic oxide particles

期刊论文

Fabrication of bimetallic Cu–Zn adsorbents with high dispersion by using confined space for gas adsorptive

期刊论文

Removing polybrominated diphenyl ethers in pure water using Fe/Pd bimetallic nanoparticles

Min ZHANG,Jian LU,Zhencheng XU,Yiliang HE,Bo ZHANG,Song JIN,Brian BOMAN

期刊论文

Dechlorination of dichlorodiphenyltrichloroethane (DDT) by Fe/Pd bimetallic nanoparticles: Comparison

Kubra Ulucan-Altuntas, Eyup Debik

期刊论文

Mechanistic understanding of Cu-based bimetallic catalysts

You Han, Yulian Wang, Tengzhou Ma, Wei Li, Jinli Zhang, Minhua Zhang

期刊论文

A Pt-Bi bimetallic nanoparticle catalyst for direct electro-oxidation of formic acid in fuel cells

Shu-Hong LI, Yue ZHAO, Jian CHU, Wen-Wei LI, Han-Qing YU, Gang LIU, Yang-Chao TIAN

期刊论文

Electrochemical CO reduction to C products over CuZn intermetallic catalysts synthesized by electrodeposition

期刊论文

Oxygen reduction electrocatalysis: From conventional to single-atomic platinum-based catalysts for proton

期刊论文

Promising approach for preparing metallic single-atom catalysts: electrochemical deposition

期刊论文