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Petroleum Science 2024年第1期21卷 674-682页

作者： Jing He Kun Zhu Wei Jiang Dong-Ao Zhu Lin-Hua Zhu Hai-Yan Huang Wen-Shuai Zhu Hua-Ming Li Institute for Energy Research Jiangsu UniversityZhenjiang212013JiangsuChina College of Chemistry and Chemical Engineering Hainan Normal UniversityKey Laboratory of Water Pollution Treatment and Resource Reuse of Hainan ProvinceHaikou571158HainanChina

Synergic catalytic effect between active sites and supports greatly determines the catalytic activity for the aerobic oxidative desulfurization of fuel oils.In this work,Ni-doped Co-based Bimetallic metal-organic framework(CoNi-MOF)is fabricated to disperse N-hydroxyphthalimide(NHPI),in which the whole catalyst provides plentiful synergic catalytic effect to improve the performance of oxidative desulfurization(ODS).As a Bimetallic MOF,the second metal Ni doping results in the flower-like morphology and the modification of electronic properties,which ensure the exposure of NHPI and strengthen the synergistic effect of the overall catalyst.Compared with the monometallic Co-MOF and naked NHPI,the NHPI@CoNi-MOF triggers the efficient activation of molecular oxygen and improves the ODS performance without an initiator.The sulfur removal of dibenzothiophene-based model oil reaches 96.4%over the NHPI@CoNi-MOF catalyst in 8 h of reaction.Furthermore,the catalytic product of this aerobic ODS reaction is sulfone,which is adsorbed on the catalyst surface due to the difference in polarity.This work provides new insight and strategy for the design of a strong synergic catalytic effect between NHPI and Bimetallic supports toward high-activity aerobic ODS materials.

关键词： Metal-organic frameworks Doped Bimetallic N-hydroxyphthalimide Aerobic processes Oxidative desulfurization

Bimetallic clusters confined inside silicalite-1 for stable propane dehydrogenation

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Nano Research 2023年第8期16卷 10881-10889页

作者： Xueer Wei Jiawei Cheng Yubing Li Kang Cheng Fanfei Sun Qinghong Zhang Ye Wang State Key Laboratory of Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy MaterialsCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361005China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201800China Shanghai Institute of Applied Physics Chinese Academy of SciencesShanghai 201204China

The noble metal-based Bimetallic clusters with high atom utilization and surface energy have been widely applied in heterogeneous catalysis,but the stabilization of these metastable clusters in harsh reaction conditions is quite challenging.Herein,we synthesize a series of Pt-,Pd-,and Ru-based clusters promoted by a second non-noble metal(Zn,Cu,Sn,and Fe),which are confined inside silicalite-1(pure silica,S-1)crystals by a ligand-protected method.The second metal could well stabilize and disperse the noble atoms inside the rigid S-1 zeolites via Si–O–M bonds,thus enabling to lower the usage of expensive noble metals in catalysts.The as-synthesized Bimetallic catalysts exhibited excellent performance in non-oxidative propane dehydrogenation(PDH)reaction,which is typically operated above 500℃.The PtZn@S-1,PtCu@S-1,and PtSn@S-1 with only a~0.17 wt.%Pt loading offer a significant enhancement in PDH performance compared with the conventional PtSn/Al_(2)O_(3)catalyst with a 0.5 wt.%Pt loading prepared by impregnation method.Notably,the PtSn@S-1 provides a propane conversion of 45%with a 99%propylene selectivity at 550℃,close to the thermodynamic equilibrium.Furthermore,the PtSn@S-1 exhibits excellent stability during 300 h on stream and high tolerance to regeneration by a simple calcination step.

关键词： zeolite noble metal Bimetallic confinement alkane conversion

Construction of Bimetallic Pt-Pd/CeO_(2)-ZrO_(2)-La_(2)O_(3) catalysts with different Pt/Pd ratios and its structure-activity correlations for three-way catalytic performance

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Journal of Rare Earths 2023年第6期41卷 896-904,I0004页

作者： Kai Chen Jie Wan Ting Wang Qi Sun Renxian Zhou Institute of Catalysis Zhejiang UniversityHangzhou 310028China Energy Research Institute Nanjing Institute of TechnologyNanjing 211167China School of Environmental Engineering Nanjing Institute of TechnologyNanjing 211167China

A series of Pt-Pd Bimetallic catalysts supported on CeO_(2)-ZrO_(2)-La_(2)O_(3) mixed oxides were synthesized through the conventional impregnation method.Three-way catalytic performance evaluations along with detailed physio-chemical characterizations were carried out to establish possible structure-activity correlations.Results show that on the one hand,different Pt/Pd ratios can strongly affect the TWC behaviors of Pt-Pd/CZL catalysts by modulating the synergistic effect between Pt and Pd.On the other hand,higher Pt/Pd ratio also favors better dispersion of precious metals.Such improved precious metals(PM)dispersion can promote the metal-support interaction and increase the surface oxygen vacancies concentration,thereby raising the dynamic oxygen storage/release capacity,improving the redox ability as well as enha ncing the thermal stability of the Pt-Pd/CZL catalyst.Moreover,the stro ng metal-support interaction can augment surface oxygen vacancy concentration,thereby benefiting low temperature CO and NO reaction via augmented NOxadsorption and nitrate conversion.

关键词： Three-way catalyst Bimetallic Metal-support interaction Dispersion Dynamic oxygen storage/release capacity Rare earths

Parameters Affecting the Fuel Cell Reactions on Platinum Bimetallic Nanostructures

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Electrochemical Energy Reviews 2023年第1期6卷 830-853页

作者： Nicolas Alonso‑Vante IC2MP UMR-CNRS 7285University of Poitiers4 rue Michel Brunet86072 PoitiersFrance

In this paper the electrochemical properties of some platinum-based nanoalloys are reviewed.The revision is centered on electrocatalytic materials generated via the carbonyl chemical route(CCR).In considering the effects of segregation in these bimetals,the reaction of the hydrogen oxidation(HOR)and oxygen reduction(ORR)in the alkaline medium was investigated.The reaction kinetics of these electrochemical processes in the alkaline electrolyte is still a challenge.For the design of high-performance platinum-based electrocatalysts,it is of importance to know that the kinetics of HOR and ORR also depends on the Pt adsorbate.The electrochemical analysis,based on the study of Pt nanoalloyed surfaces with different Pt-adsorbate interactions,was taken into account.A clear trend in the HOR as well as the ORR activity,in the alkaline electrolyte,was established,revealing that the activity changes in the order PtSn/C

关键词： Electrocatalysts HOR HER ORR Pt-based materials Bimetallic Carbon domains

Nanostructured Bimetallic Zn/Co in N-doped carbon as an efficient catalyst for the alcohol dehydrogenation to carboxylic acids under solvent-free conditions

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Journal of Materials Science & Technology 2023年第30期161卷 111-122页

作者： Zhong-Hui Zheng Somboon Chaemchuen Jun-Fei Gu Jing Hang Wei Sang Ji-Chao Wang Ye Yuan Cheng Chen State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China School of Materials Science and Engineering Wuhan University of TechnologyWuhan 430070China

The catalytic alcohol dehydrogenation to carboxylic acids has been demonstrated as an atom-economic and environmental-friendly synthetic method.However,the reported catalysts either require relatively complicated synthesis or exhibit high activity only in the presence of a solvent.Therefore,it is still in high demand to obtain catalysts that feature facile synthesis and perform well even without any solvent.Herein,a series of nanostructured Bimetallic Zn/Co species embedded in N-doped hierarchical porous carbon were fabricated in a facile and green manner.More significantly,the best-performing material(Zn/Co@NC-800)was identified as the first heterogeneous catalyst to enable this transformation under solvent-free conditions.Moreover,the as-prepared composites were comprehensively investigated to de-termine their structural and morphological properties,which rationalized the superiority of Zn/Co@NC-800 over the other synthesized materials.Further studies signified that Co sites(both Co^(0)and Co^(2+))and N species(mainly pyridinic N)were probably involved in this process,functioning as the Lewis acid site and basic site,respectively.Hopefully,this study could provide a simple and sustainable method for carboxylic acid synthesis.

关键词： Heterogeneous catalysis Bimetallic ZIFs Pyrolysis Solvent-free Alcohol dehydrogenation Carboxylic acids

Dechlorination of dichlorodiphenyltrichloroethane(DDT)by Fe/Pd Bimetallic nanoparticles:Comparison with nZVI?degradation mechanism,and pathways

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Frontiers of Environmental Science & Engineering 2020年第1期14卷 199-211页

作者： Kubra Ulucan-Altuntas Eyup Debik Civil Engineering Faculty Environmental Engineering DepartmentYildiz Technical UniversityIstanbul 34220Turkey

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.Dichlorodiphcnyltrichloroethane(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,0.23μg/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

Ligand-mediated contaminant degradation by bare and carboxymethyl cellulose-coated Bimetallic palladium-zero valent iron nanoparticles in high salinity environments

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Journal of Environmental Sciences 2019年第3期31卷 303-311页

作者： Xiaoming Ma Di He Adele M.Jones T.David Waite Taicheng An Institute of Environmental Health and Pollution Control Guangdong University of Technology Guangzhou Key Laboratory of Environmental Catalysis and Pollution Control School of Environmental Science and Engineering Guangzhou University of Technology School of Civil and Environmental Engineering University of New South Wales

The application of nanoscale zero-valent iron(nZVI) for the degradation of contaminants has been extensively investigated, however, few studies have focused on degradation in high salinity environments. In this study, the ability of bare and carboxymethyl cellulose(CMC)-coated Bimetallic Pd-nZVI particles to degrade 33′44′-tetrachlorobiphenyl in high saline water(SW) is examined with particular attention given to the effects of ethylenediaminetetraacetic acid(EDTA) on the rate of degradation. EDTA enhances the reactivity of Pd-nZVI in SW, with evidence provided to link this to the removal of the passivating layer. Additionally, a conceptual model is proposed which provides a quantitative description of the removal of these iron oxide layers in the presence of EDTA. An optimum EDTA to bare Pd-nZVI molar ratio of 0.1 exists, with insufficient EDTA unable to remove the passivating layer whilst excess EDTA results in Fe loss and enhanced agglomeration due to magnetic attraction of the bare Fe(0) particles. In contrast, CMCcoating of Pd-nZVI assemblages actually impedes degradation, despite the coated particles displaying a smaller average size compared to uncoated particles, with even the presence of EDTA in this case not significantly improving degradation. The reduced reactivity in the presence of CMC is primarily attributed to the effect of CMC on the association of Pd with nZVI particles. In particular, the presence of CMC reduced the total amount of Pd incorporated with the stabilized particles compared to the non-stabilized particles.Additionally, the presence of CMC results in less Pd present in its reactive zero-valent oxidation state.

关键词： Bimetallic zero valent iron ligand-mediated depassivation polychlorinated biphenyls high salinity water

Performance of Ni-Cu Bimetallic co-catalyst g-C3N4 nanosheets for improving hydrogen evolution

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Journal of Materials Science & Technology 2020年第14期47卷 144-156页

作者： Zhiliang Jin Lijun Zhang School of Chemistry and Chemical Engineering North Minzu UniversityYinchuan 750021China Ningxia Key Laboratory of Solar Chemical Conversion Technology North Minzu UniversityYinchuan 750021China Key Laboratory for Chemical Engineering and Technology State Ethnic Affairs CommissionNorth Minzu UniversityYinchuan 750021China

The Ni-Cu Bimetallic nanoparticles were successfully anchorred on the surface of g-C3N4 nanosheets by a simple heat treatment process which was applied to the photocatalytic hydrogen evolution reaction.Insitu introduction of Ni-Cu could significantly improve the photocatalytic hydrogen evolution performance compared with pure g-C3N4 in the system sensitized by eosin Y under a visible irradiation condition.The hydrogen production activity of the composite reached 104.4μmol(2088.28μmol g^-1 h^-1)after using the Ni Cu double promoter strategy,which was 24.3 times higher than g-C3N4.The excellent electrical conductivity of the Bimetallic Ni-Cu and the close interfacial contact between Ni Cu and g-C3N4 played an important role for increasing the charge transfer rate.They were also the reasons of more efficient charge separation,which ultimately led to a significant promotion on the photocatalytic hydrogen production reaction.Ni-Cu/g-C3N4 coupling with a close Schottky interface between metal and semiconductor which enhanced H2-evolution performance and TEOA oxidation kinetics.This work provided a new way to load Ni Cu Bimetallic nanoparticles in situ onto g-C3N4 and a reference on relative semiconductor materials.

关键词： Bimetallic Ni-Cu g-C3N4 Charge separation Hydrogen evolution

Effect of preparation method on the Bimetallic NiCu/SAPO-11 catalysts for the hydroisomerization of n-octane

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Journal of Energy Chemistry 2019年第1期28卷 23-30页

作者： Zhichao Yang Yunqi Liu Yanpeng Li Lingyou Zeng Zhi Liu Xueying Liu Chenguang Liu State Key Laboratory of Heavy Oil Processing Key Laboratory of Catalysis China National Petroleum Corp. (CNPC) China University of Petroleum (East China)

The Bimetallic NiCu/SAPO-11 catalysts were prepared by co-impregnation, sequential impregnation, coprecipitation, and mechanical mixing methods. Powder X-ray diffraction, nitrogen adsorption-desorption,temperature-programmed desorption of ammonia, transmission electron microscopy, temperatureprogrammed reduction of hydrogen, and X-ray photoelectron spectroscopy were used to characterize the physicochemical properties of the catalysts. The catalytic performance of the catalysts was assessed by the hydroisomerization of n-octane. Results indicated that the conversion of n-octane and selectivity to n-octane isomers were related to the preparation methods of the catalysts. The catalysts with Ni-Cu alloy effectively restrained the hydrogenolysis reaction that decreases the selectivity of isomerization. The catalyst prepared by the mechanical mixing of NiO and CuO hardly formed Ni-Cu alloy, showing obvious hydrogenolysis and low selectivity to n-octane isomers. The unbalance between the metal and acid sites resulted in the low conversion of n-octane and selectivity to n-octane isomers. Among all the catalysts,the catalyst prepared by the co-impregnation method exhibited high catalytic activity and selectivity to n-octane isomers.

关键词： Ni-Cu/SAPO-11 Bimetallic Preparation method Hydroisomerization Hydrogenolysis n-Octane

Identifying the composition and atomic distribution of Pt-Au Bimetallic nanoparticle with machine learning and genetic algorithm

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Chinese Chemical Letters 2020年第3期31卷 890-896页

作者： Jiawei Zhang Jianfu Chen Peijun Hu Haifeng Wang Key Laboratory for Advanced Materials Research Institute of Industrial Catalysis and Centre for Computational ChemistrySchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China School of Chemistry and Chemical Engineering The Queen's University of BelfastBelfast BT95AGUnited Kingdom

Bimetallic nanoparticles(AmBn)usually exhibit rich catalytic chemistry and have drawn tremendous attention in heterogeneous catalysis.However,challenged by the huge configuration space,the understanding toward their composition and distribution of A/B element is known little at the atomic level,which hinders the rational synthesis.Herein,we develop an on-the-fly training strategy combing the machine learning model(SchNet)with the genetic algorithm(GA)search technique,which achieve the fast and accurate energy prediction of complex Bimetallic clusters at the DFT level.Taking the 38-atom PtmAu38-mnanoparticle as example,the element distribution identification problem and the stability trend as a function of Pt/Au composition is quantitatively re solved.Specifically,results show that on the Pt-rich cluster Au atoms prefer to occupy the low-coordinated surface corner sites and form patch-like surface segregation patte rns,while for the Au-rich ones Pt atoms tend to site in the co re region and form the co re-shell(Pt@Au)configuration.The thermodynamically most stable PtmAu38-mcluster is Pt6 Au32,with all the core-region sites occupied by Pt,rationalized by the stronger Pt-Pt bond in comparison with Pt-Au and Au-Au bonds.This work exemplifies the potent application of rapid global sea rch enabled by machine learning in exploring the high-dimensional configuration space of Bimetallic nanocatalysts.

关键词： Density functional theory calculation Machine learning Genetic algorithm Bimetallic nanoparticle PtAu cluster