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

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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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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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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Recent advances in selective acetylene hydrogenation using palladium containing catalysts

Alan J. McCue, James A. Anderson

《化学科学与工程前沿（英文）》 2015年 第9卷 第2期   页码 142-153 doi: 10.1007/s11705-015-1516-4

摘要： Recent advances with Pd containing catalysts for the selective hydrogenation of acetylene are described. The overview classifies enhancement of catalytic properties for monometallic and bimetallic Pd catalysts. Activity/selectivity of Pd catalysts can be modified by controlling particle shape/morphology or immobilisation on a support which interacts strongly with Pd particles. In both cases enhanced ethylene selectivity is generally associated with modifying ethylene adsorption strength and/or changes to hydride formation. Inorganic and organic selectivity modifiers (i.e., species adsorbed onto Pd particle surface) have also been shown to enhance ethylene selectivity. Inorganic modifiers such as TiO change Pd ensemble size and modify ethylene adsorption strength whereas organic modifiers such as diphenylsulfide are thought to create a surface template effect which favours acetylene adsorption with respect to ethylene. A number of metals and synthetic approaches have been explored to prepare Pd bimetallic catalysts. Examples where enhanced selectivity is observed are generally associated with decreased Pd ensemble size and/or hindering of the ease with which an unselective hydride phase is formed for Pd. A final class of bimetallic catalysts are discussed where Pd is not thought to be the primary reaction site but merely acts as a site where hydrogen dissociation and spillover occurs onto a second metal (Cu or Au) where the reaction takes place more selectively.

关键词： acetylene     ethylene     selective hydrogenation     palladium     bimetallic    

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Pd nano-catalyst supported on biowaste-derived porous nanofibrous carbon microspheres for efficient catalysis

《化学科学与工程前沿（英文）》 2023年 第17卷 第9期   页码 1289-1300 doi: 10.1007/s11705-023-2299-7

摘要： Environmental pollution caused by the presence of aromatic aldehydes and dyes in wastewater is a serious global concern. An effective strategy for the removal of these pollutants is their catalytic conversion, possibly to valuable compounds. Therefore, the design of efficient, stable and long-lifetime catalysts is a worthwhile research goal. Herein, we used nanofibrous carbon microspheres (NCM) derived from the carbohydrate chitin present in seafood waste, and characterized by interconnected nanofibrous networks and N/O-containing groups, as carriers for the manufacture of a highly dispersed, efficient and stable Pd nano-catalyst (mean diameter ca. 2.52 nm). Importantly, the carbonised chitin’s graphitized structure, defect presence and large surface area could promote the transport of electrons between NCM and Pd, thereby endowing NCM supported Pd catalyst with high catalytic activity. The NCM supported Pd catalyst was employed in the degradation of some representative dyes and the chemoselective hydrogenation of aromatic aldehydes; this species exhibited excellent catalytic activity and stability, as well as applicability to a broad range of aromatic aldehydes, suggesting its potential use in green industrial catalysis.

关键词： biowaste chitin     nanofibrous     palladium     nano-catalyst     catalysis    

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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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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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2-Aminopyridine functionalized cellulose based Pd nanoparticles: An efficient and ecofriendly catalyst

Peibo Hu,Yahao Dong,Xiaotian Wu,Yuping Wei

《化学科学与工程前沿（英文）》 2016年 第10卷 第3期   页码 389-395 doi: 10.1007/s11705-016-1575-1

摘要： A palladium catalyst supported on 2-aminopyridine functionalized cellulose was synthesized and fully characterized by inductively coupled plasma atomic emission spectroscopy, transmission electron microscope, Fourier transform infrared spectroscopy, thermogravimetric analysis and X-ray photoelectron spectrometry. This catalyst can be applied in the Suzuki cross-coupling reaction of aryl halides with arylboronic acids in 50% ethanol to afford biaryls in?good yields, and easily recycled by simple filtration after reaction without the loss of metal Pd.

关键词： cellulose-supported     2-aminopyridine     palladium nanoparticles     ecofriendly catalyst     Suzuki cross-coupling reaction    

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Tailoring the simultaneous abatement of methanol and NO on Sb-Ce-Zr catalysts via copper modification

《环境科学与工程前沿（英文）》 2022年 第16卷 第10期 doi: 10.1007/s11684-022-1565-0

摘要：

● Cu addition enhances CH3OH oxidation and alleviates its inhibitory effect on SCR.

关键词： Copper modification     Sb-CeZr2Ox catalyst     NOx     Methanol     Simultaneous removal    

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Biogenic palladium prepared by activated sludge microbes for the hexavalent chromium catalytic reduction

Luman Zhou, Chengyang Wu, Yuwei Xie, Siqing Xia

《环境科学与工程前沿（英文）》 2020年 第14卷 第2期 doi: 10.1007/s11783-019-1206-4

摘要： • Pd nanoparticles could be reduced and supported by activated sludge microbes. • The effect of biomass on Pd adsorption by microbes is greater than Pd reduction. • More biomass reduces Pd particle size, which is more dispersed on the cell surface. • When the biomass/Pd add to 6, the catalytic reduction rate of Cr(VI) reaches stable. Palladium, a kind of platinum group metal, owns catalytic capacity for a variety of hydrogenations. In this study, Pd nanoparticles (PdNPs) were generated through enzymatic recovery by microbes of activated sludge at various biomass/Pd, and further used for the Cr(VI) reduction. The results show that biomass had a strong adsorption capacity for Pd(II), which was 17.25 mg Pd/g sludge. The XRD and TEM-EDX results confirmed the existence of PdNPs associated with microbes (bio-Pd). The increase of biomass had little effect on the reduction rate of Pd(II), but it could cause decreasing particle size and shifting location of Pd(0) with the better dispersion degree on the cell surface. In the Cr(VI) reduction experiments, Cr(VI) was first adsorbed on bio-Pd with hydrogen and then reduced using active hydrogen as electron donor. Biomass improved the catalytic activity of PdNPs. When the biomass/Pd (w/w) ratio increased to six or higher, Cr(VI) reduction achieved maximum rate that 50 mg/L of Cr(VI) could be rapidly reduced in one minute.

关键词： Palladium nanoparticles     Activated sludge     Hexavalent chromium    

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Effect of alkyl nitrite decomposition on catalytic performance of CO coupling reaction over supported palladiumcatalyst

Zhenhua LI, Weihan WANG, Dongxue YIN, Jing LV, Xinbin MA

《化学科学与工程前沿（英文）》 2012年 第6卷 第4期   页码 410-414 doi: 10.1007/s11705-012-1213-5

摘要： The syntheses of dimethyl oxalate (DMO) and diethyl oxalate (DEO) by CO coupling reaction in gaseous phase were investigated in a fixed bed reactor over Pd-Fe/Al O catalyst. The catalytic performance was characterized by CO conversion, space-time yield (STY) and selectivity of DMO (or DEO). The results showed that over Pd-Fe/Al O catalyst, the STY of DMO was higher than that of DEO under the same reaction conditions. The optimum reaction temperatures for synthesizing DMO and DEO were 403 K and 393 K, respectively, at the molar ratio 1 ∶ 1 of alkyl nitrite to CO. The difference in synthesizing DMO and DEO on the same catalyst was attributed to the decomposition performances of methyl nitrite (MN) and ethyl nitrite (EN), as density functional theory (DFT) calculation showed that EN decomposed more easily than MN.

关键词： palladium     CO coupling     dialkyl oxalate     alkyl nitrite     decomposition    

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Preparation and investigation of Pd doped Cu catalysts for selective hydrogenation of acetylene

Xinxiang Cao, Tengteng Lyu, Wentao Xie, Arash Mirjalili, Adelaide Bradicich, Ricky Huitema, Ben W.-L. Jang, Jong K. Keum, Karren More, Changjun Liu, Xiaoliang Yan

《化学科学与工程前沿（英文）》 2020年 第14卷 第4期   页码 522-533 doi: 10.1007/s11705-019-1822-3

摘要： A series of PdCu bimetallic catalysts with low Cu and Pd loadings and different Cu: Pd atomic ratios were prepared by conventionally sequential impregnation (CSI) and modified sequential impregnation (MSI) of Cu and Pd for selective hydrogenation of acetylene. Characterization indicates that the supported copper (II) nitrate in the PdCu bimetallic catalysts prepared by MSI can be directly reduced to Cu metal particles due to the hydrogen spillover from Pd to Cu(NO ) crystals. In addition, for the catalysts prepared by MSI, Pd atoms can form PdCu alloy on the surface of metal particles, however, for the catalysts prepared by CSI, Pd tends to migrate and exist below the surface layer of Cu. Reaction results indicate that compared with CSI, the MSI method enables samples to possess preferable stability as well as comparable reaction activity. This should be due to the MSI method in favor of the formation of PdCu alloy on the surface of metal particles. Moreover, even Pd loading is super low,<0.045 wt-% in this study, by through adjusting Cu loading to an appropriate value, attractive reactivity and selectivity still can be achieved.

关键词： copper     palladium     catalysts     acetylene     selective hydrogenation    

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Experimental research on thermal transport properties of crystallized palladium-based alloys

Siyuan CHENG, Xuguo SHI, Weigang MA, Xing ZHANG, Guanglai LIU, Mingxiang PAN, Weihua WANG

《能源前沿（英文）》 2018年 第12卷 第1期   页码 121-126 doi: 10.1007/s11708-018-0531-9

摘要： Palladium-based alloy is a kind of material with a high glass forming ability and can be easily formed into an amorphous state. After an annealing process, it can also be maintained at a crystallized state. To study the thermal and electrical transport properties of crystallized palladium-based alloys, the steady-state T-type method, standard four-probe method, and AC heating-DC detecting T-type method were used to measure the thermal conductivity, electrical conductivity, and Seebeck coefficient of crystallized Pd Ni Cu P and Pd Ni Cu P alloys respectively. The results show that compared to amorphous samples, the thermal conductivity and electrical conductivity of crystallized palladium-based alloys are significantly higher, while the Seebeck coefficient is lower. The ratio of crystallized and amorphous thermal conductivity is higher for Pd Ni Cu P alloy fiber which has a higher glass forming ability, while the ratio of electronic thermal conductivity almost remains constant for both alloy fibers. The results also show that the slope of electrical resistivity to temperature is a function of elemental composition for crystallized quaternary palladium-based alloy fibers. The sensitivity of thermal conductivity and electrical conductivity to the composition is high, while the correlation between Seebeck coefficient and composition is relatively weak.

关键词： palladium-based alloy     T-type method     thermal conductivity     electrical conductivity     Seebeck coefficient    

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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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Copolymerization of polyketones catalyzed by polyacrylonitrile resin-supported palladium acetate

GUO Jintang, ZHANG Hongxin, WANG Bo, YE Yaqin

《化学科学与工程前沿（英文）》 2008年 第2卷 第2期   页码 165-170 doi: 10.1007/s11705-008-0010-7

摘要： The crosslinked polyacrylonitrile (PAN) was synthesized by suspension polymerization using acrylonitrile (ANT) and divinylbenzene (DVB). Effects of a variety of conditions on the polymerization of PAN particle size and stiffness were investigated. Polyketone was prepared by the copolymerization of carbon monoxide (CO) and styrene (ST) catalyzed by PAN resin-supported palladium acetate. The resin-supported catalyst and the copolymerization product were characterized by infrared spectroscopy (IR) and Scanning Electron Microscopy (SEM). Effects of the components of a catalytic system and reaction time on the catalytic activity were studied. The reusability of the resin-supported catalyst was also investigated. Results indicated that the resin-supported catalyst has excellent catalytic property. The yield of polyketone was 6.2348 g when using 1 g of resin and 22.4 mg of palladium acetate.

关键词： copolymerization     Electron Microscopy     monoxide     excellent catalytic     Polyketone    

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标题 作者 时间 类型 操作

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

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

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

Ni-Co bimetallic catalyst for CH

Xiaohong LI, Jun AI, Wenying LI, Dongxiong LI

期刊论文

Recent advances in selective acetylene hydrogenation using palladium containing catalysts

Alan J. McCue, James A. Anderson

期刊论文

Pd nano-catalyst supported on biowaste-derived porous nanofibrous carbon microspheres for efficient catalysis

期刊论文

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

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

2-Aminopyridine functionalized cellulose based Pd nanoparticles: An efficient and ecofriendly catalyst

Peibo Hu,Yahao Dong,Xiaotian Wu,Yuping Wei

期刊论文

Tailoring the simultaneous abatement of methanol and NO on Sb-Ce-Zr catalysts via copper modification

期刊论文

Biogenic palladium prepared by activated sludge microbes for the hexavalent chromium catalytic reduction

Luman Zhou, Chengyang Wu, Yuwei Xie, Siqing Xia

期刊论文

Effect of alkyl nitrite decomposition on catalytic performance of CO coupling reaction over supported palladiumcatalyst

Zhenhua LI, Weihan WANG, Dongxue YIN, Jing LV, Xinbin MA

期刊论文

Preparation and investigation of Pd doped Cu catalysts for selective hydrogenation of acetylene

Xinxiang Cao, Tengteng Lyu, Wentao Xie, Arash Mirjalili, Adelaide Bradicich, Ricky Huitema, Ben W.-L. Jang, Jong K. Keum, Karren More, Changjun Liu, Xiaoliang Yan

期刊论文

Experimental research on thermal transport properties of crystallized palladium-based alloys

Siyuan CHENG, Xuguo SHI, Weigang MA, Xing ZHANG, Guanglai LIU, Mingxiang PAN, Weihua WANG

期刊论文

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

期刊论文

Copolymerization of polyketones catalyzed by polyacrylonitrile resin-supported palladium acetate

GUO Jintang, ZHANG Hongxin, WANG Bo, YE Yaqin

期刊论文