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Differentially-grown cobalt regulators cooperatively involved in the tandem catalysis for high-yield production of second amines

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Nano Research 2024年第4期17卷 2444-2450页

作者： Jinhui Xu Xiao Wang Ying Wang Fei Wang Lingling Zhang Wenjie Cui Shuyan Song Hongjie Zhang State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026China Department of Chemistry Tsinghua UniversityBeijing 100084China

One-pot tandem catalysis has been regarded as one of the most atomic economic ways to produce secondary amines,the important platform molecules for chemical synthesis and pharmaceutical manufacture,but it is facing serious issues in overall *** promotional effects are highly desired for boosting the activity and regulating the selectivity of conventional tandem *** this work,we report a high-performance tandem catalyst with maximized synergistic effect among each counterpart by preciously manipulating the spatial structure,which involves the active CeO_(2)/Pt component as kernel,the densely-coated N-doped C(NC)layer as selectivity controller,and the differentially-grown Co species as catalytic performance *** comprehensive investigations,the unique growth mechanism and the promotion effect of Co regulators are ***,the surface-landed Co clusters(Cocs)are crucial to selectivity by altering the adsorption configuration of benzylideneaniline ***,the inner Co particles(Cops)are essential for activity by denoting their electrons to neighboring *** from the unique promotion effect,a remarkably-improved catalytic efficiency(100%nitrobenzene conversion with 94%N-benzylaniline selectivity)is achieved at a relatively low temperature of 80℃,which is much better than that of CeO_(2)/Pt(100%nitrobenzene conversion with 12%N-benzylaniline selectivity)and CeO_(2)/Pt/NC(35%nitrobenzene conversion with 94%benzylideneaniline selectivity).

关键词： tandem catalysis CeO_(2) hierarchical structure heterogeneous catalyst dual-site materials

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One-Pot Upgrading Polyethylene and CO_(2)to Aromatics via tandem catalysis

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CCS Chemistry 2024年第6期6卷 1422-1429页

作者： Wenjun Chen Yuchen Jiao Yue Liu Meng Wang Fan Zhang Ding Ma National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan) College of ChemistrySichuan UniversityChengdu 610064Sichuan Beijing National Laboratory for Molecular Sciences New Cornerstone Science LaboratoryCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871

Polyolefins have the largest share in plastic waste,so it is vital to transform these end-of-life wastes into highly valued *** present here a new catalytic method to produce aromatics using PE as a carbon *** results indicate that polyethylene(PE)and CO_(2)can be converted into aromatics and CO simultaneously,achieving a high transformation rate and a 64.0%selectivity toward aromatics below 400℃ by Cu-Fe_(3)O_(4)and Zn/ZSM-5 tandem ***,the established theoretical limit of 50%selectivity toward aromatics in PE aromatization is *** is attributed to the coexistence of reverse water-gas shift,which converts another feed,CO_(2),with hydrogen to produce valuable CO,confirmed by^(13)C isotope *** consumes excessive hydrogen generated during PE aromatization to produce CO and mitigates the production of light alkanes from hydrogen transfer reactions,thereby augmenting the formation of aromatic *** research offers a new approach to valorizing two prevalent waste carbon sources:waste plastic and CO_(2),which is useful for designing a new strategy for upcycling waste carbon resources.

关键词： polyethylene CO_(2) tandem catalysis upgrading aromatics

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tandem catalysis for enhanced CO oxidation over the Bi-Au-SiO_(2)interface

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Nuclear Science and Techniques 2023年第7期34卷 198-205页

作者： Huan Zhang Lei Xie Zhao-Feng Liang Chao-Qin Huang Hong-Bing Wang Jin-Ping Hu Zheng Jiang Fei Song Instrumentation and Service Center for Physical Sciences Westlake UniversityHangzhou 310024China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China Shanghai Institute of Applied Physics Chinese Academy of SciencesShanghai 201800China

Bimetallic catalysts typically exploit unique synergetic effects between two metal species to achieve their catalytic *** the mechanism of CO oxidation using hybrid heterogeneous catalysts is important for effective catalyst design and environmental ***,we report a Bi-Au/SiO_(2)tandem bimetallic catalyst for the oxidation of CO over the Au/SiO_(2)surface,which was monitored using near-ambient-pressure X-ray photoelectron *** Au-decorated SiO_(2)catalyst exhibited scarce activity in the CO oxidation reaction;however,the introduction of Bi to the Au/SiO_(2)system promoted the catalytic *** mechanism is thought to involve the dissociation O_(2)molecules in the presence of Bi,which results in spillover of the O species to adjacent Au atoms,thereby forming Au^(δ+).Further CO adsorption,followed by thermal treatment,facilitated the oxidation of CO at the Au-Bi interface,resulting in a reversible reversion to the neutral Au valence *** work provides insight into the mechanism of CO oxidation on tandem surfaces and will facilitate the rational design of other Au-based catalysts.

关键词： APXPS CO oxidation Au-Bi interface tandem catalysis In situ

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tandem catalysis on adjacent active motifs of copper grain boundary for efficient CO_(2) electroreduction toward C2 products

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Journal of Energy Chemistry 2022年第7期31卷 219-223,I0006页

作者： Tao Luo Kang Liu Junwei Fu Shanyong Chen Hongmei Li Junhua Hu Min Liu Hunan Joint International Research Center for Carbon Dioxide Resource Utilization State Key Laboratory of Powder MetallurgySchool of Physics and ElectronicsCentral South UniversityChangsha 410083HunanChina School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450002HenanChina

Copper (Cu) is a special electrocatalyst for CO_(2) reduction reaction (CO_(2)RR) to multi-carbon *** introducing grain boundaries (GBs) into Cu-based catalysts is an efficient strategy to improve the selectivity of C^(2+) ***,it is still elusive for the C^(2+) product generation on Cu GBs due to the complex active *** this work,we found that the tandem catalysis pathway on adjacent active motifs of Cu GB is responsible for the enhanced activity for C^(2+)production by first principles *** electronic structure analysis shows,the d-band center of GB site is close to the Fermi level than Cu(100) facet,the Cu atomic sites at grain boundary have shorter bond length and stronger bonding with*CO,which can enhance the adsorption of*CO at GB ***,CO_(2)protonation is more favorable on the region Ⅲ motif (0.84 e V) than at Cu(100) site (1.35 e V).Meanwhile,the region Ⅱ motif also facilitate the C–C coupling (0.72 e V) compared to the Cu(100) motif (1.09 e V).Therefore,the region Ⅲ and Ⅱ motifs form a tandem catalysis pathway,which promotes the C^(2+)selectivity on Cu *** work provides new insights into CO_(2)RR process.

关键词： Cu(100)facet Grain boundary CO_(2)electroreduction C2+products tandem catalysis

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In situ reconstruction induced oxygen-deficient multiphase Cu based species hybridized with Ni single atoms as tandem platform for CO_(2) electroreduction

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Nano Research 2024年第5期17卷 3888-3894页

作者： Juzhe Liu Yuheng Wang Pengpeng Mo Feng Yang Kaiqi Jiang Zhixiang Cheng Yuxuan Liu Zhiyi Sun Zheng Liu Yimei Zhang Wenxing Chen The Key Laboratory of Resources and Environmental System Optimization Ministry of EducationCollege of Environmental Science and EngineeringNorth China Electric Power UniversityBeijing 102206China Energy&catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijing 100012China SEPA Key Laboratory of Eco-Industry Chinese Research Academy of Environmental SciencesBeijing 100012China

tandem catalysis,capable of decoupling individual steps,provides a feasible way to build a high-efficiency CO_(2) electro-conversion system for multicarbons(C_(2+)).The construction of electrocatalytic materials is one of focusing ***,we fabricated a single atom involved multivalent oxide-derived Cu composite material and found it inclined to reconstruct into oxygen-deficient multiphase Cu based species hybridized with monatomic Ni on N doped C *** this prototype,rapid CO generation and C-C coupling are successively achieved on NiN4 sites and surface amorphized Cu species with defects,resembling a micro-production *** this way,the in situ formed tandem catalyst exhibited a high Faradaic efficiency(FE)of~78%for C_(2+)products along with satisfactory durability over 50 ***,the reconstruction-induced amorphous layer with abundant asymmetric sites should be favorable to improve the ethanol selectivity(FE:63%),which is about 10 times higher than that of the non-tandem Cu-based contrast *** work offers a new approach for manipulating tandem catalyst systems towards enhancing C_(2+)products.

关键词： tandem catalysis single atom reconstruction amorphous CO_(2)reduction reaction

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Bismuth clusters pinned on TiO_(2) porous nanowires boosting charge transfer for CO_(2) photoreduction to CH_(4)

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Nano Research 2024年第3期17卷 1190-1198页

作者： Jiazhi Meng Kaiwen Wang Yang Wang Jiangping Ma Chaogang Ban Yajie Feng Bin Zhang Kai Zhou Liyong Gan Guang Han Danmei Yu Xiaoyuan Zhou College of Physics and Institute of Advanced Interdisciplinary Studies Chongqing UniversityChongqing 401331China School of Chemistry and Chemical Engineering Chongqing UniversityChongqing 401331China College of Materials Science and Engineering Chongqing UniversityChongqing 400044China Beijing Key Lab of Microstructure and Properties of Advanced Materials Beijing University of TechnologyBeijing 100124China Analytical and Testing Center Chongqing UniversityChongqing 401331China

Artificial photosynthesis in carbon dioxide(CO_(2))conversion into value-added chemicals attracts considerable attention but suffers from the low activity induced by sluggish separation of photogenerated carriers and the kinetic bottleneck-induced unsatisfied ***,we prepare a new-style Bi/TiO_(2) catalyst formed by pinning bismuth clusters on TiO_(2) nanowires through being confined by pores,which exhibits high activity and selectivity towards photocatalytic production of CH_(4) from CO_(2).Boosted charge transfer from TiO_(2) through Bi to the reactants is revealed via in situ X-ray photon spectroscopy and time-resolved photoluminescence(PL).Further,in situ Fourier transform infrared results confirm that Bi/TiO_(2) not only overcomes the multi-electron kinetics challenge of CO_(2) to CH_(4) via boosting charge transfer,but also facilitates proton production and transfer as well as the intermediates*CHO and*CH_(3)O generation,ultimately achieving the tandem catalysis towards *** calculation also underlies that the more favorable reaction step from*CO to*CHO on Bi/TiO_(2) results in CH_(4) production with higher *** work brings new insights into rational design of photocatalysts with high performance and the formation mechanism of CO_(2) to CH_(4) for solar energy storage in future.

关键词： carbon dioxide(CO_(2))photoreduction charge transfer tandem catalysis methanation

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tandem Lewis acid catalysis for the conversion of alkenes to 1,2‐diols in the confined space of bifunctional TiSn‐Beta zeolite

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Chinese Journal of catalysis 2021年第7期42卷 1176-1184页

作者： Qifeng Lei Chang Wang Weili Dai Guangjun Wu Naijia Guan Michael Hunger Landong Li School of Materials Science and Engineering&National Institute for Advanced Materials Nankai UniversityTianjin 300350China Key Laboratory of Advanced Energy Materials Chemistry of the Ministry of Education Collaborative Innovation Center of Chemical Science and EngineeringNankai UniversityTianjin 300071China Institute of Chemical Technology University of StuttgartStuttgart 70550Germany

The generation of multifunctional isolated active sites in zeolite supports is an attractive method for integrating multistep sequential reactions into a single‐pass tandem catalytic *** this study,bifunctional TiSn‐Beta zeolite was prepared by a simple and scalable post‐synthesis approach,and it was utilized as an efficient heterogeneous catalyst for the tandem conversion of alkenes to 1,2‐*** isolated Ti and Sn Lewis acid sites within the TiSn‐Beta zeolite can efficiently integrate alkene epoxidation and epoxide hydration in tandem in a zeolite microreactor to achieve one‐step conversion of alkenes to 1,2‐diols with a high selectivity of>90%.Zeolite confinement effects result in high tandem rates of alkene epoxidation and epoxide hydration as well as high selectivity toward the desired ***,the novel method demonstrated herein can be employed to other tandem catalytic reactions for sustainable chemical production.

关键词： tandem catalysis Confinement effect Zeolite Alkene epoxidation Epoxide hydration

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Microfluidic assembly of WO_(3)/MoS_(2)Z-scheme heterojunction as tandem photocatalyst for nitrobenzene hydrogenation

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Rare Metals 2023年第2期42卷 484-494页

作者： Qing Wang Xuan-Xuan Cao Tao Liu Kang-Jie Wu Juan Deng Jing-Sheng Chen Yue-Ji Cai Meng-Qi Shen Chao Yu Wei-Kang Wang School of Environmental and Chemical Engineering Jiangsu University of Science and TechnologyZhenjiang212000China Department of Earth and Environmental Engineering Columbia UniversityNew YorkNY10027USA

Heterojunction-based photocatalyst plays an important role in the various heterogeneous catalyses.Z-scheme photocatalytic systems with two semiconductor materials are suitable for harvesting solar energy,while the advanced nanostructuring tools for the fabrication of Z-scheme heterojunction are ***,WO_(3)/MoS_(2)(W/M_(0.2))heterojunction composites were constructed in a microfluidic system with enhanced assembly efficiency,and the photocatalytic performance has been investigated using X-ray photoelectron spectroscopy(XPS),MottSchottky(M-S)analysis and gas chromatograph-mass spectrometer(GC-MS).In addition,in the reduction of nitrobenzene,the photogenerated hole(h^(+))oxidation of formic acid(HCOOH)provides the hydrogen source and the deposited Pd nanoparticles are enriched with photogenerated electrons for improving the transfer hydrogenation *** microfluidic-prepared tandem photocatalyst gives a meaningful guidance for the design and synthesis of heterojunction catalysts,which is promising for energy maximizing control systems.

关键词： tandem catalysis Photocatalysis Microfluidics Heterojunctions

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Tuning strategies and structure effects of electrocatalysts for carbon dioxide reduction reaction

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Chinese Journal of catalysis 2022年第7期43卷 1618-1633页

作者： Cong Liu Xuanhao Mei Ce Han Xue Gong Ping Song Weilin Xu State Key Laboratory of Electroanalytical Chemistry Jilin Province Key Laboratory of Low Carbon Chemical PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026AnhuiChina.

Carbon dioxide emissions have increased due to the consumption of fossil fuels,making the neutralization and utilization of CO_(2) a pressing *** a clean and efficient energy conversion process,electrocatalytic reduction can reduce carbon dioxide into a series of alcohols and acidic organic molecules,which can effectively realize the utilization and transformation of carbon *** review focuses on the tuning strategies and structure effects of catalysts for the electrocatalytic CO_(2) reduction reaction(CO_(2)RR).The tuning strategies for the active sites of catalysts have been reviewed from intrinsic and external *** structure effects for the CO_(2)RR catalysts have also been discussed,such as tandem catalysis,synergistic effects and confinement *** expect that this review about tuning strategies and structure effects can provide guidance for designing highly efficient CO_(2)RR electrocatalysts.

关键词： CO_(2)RR Tuning strategies Active sites regulation Structure effect tandem catalysis Synergistic effect

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Selectivity regulation of CO_(2)electroreduction on asymmetric AuAgCu tandem heterostructures

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Nano Research 2022年第9期15卷 7861-7867页

作者： Yating Zhu Zengqiang Gao Zhicheng Zhang Ting Lin Qinghua Zhang Huiling Liu Lin Gu Wenping Hu Tianjin Key Laboratory of Molecular Optoelectronic Sciences Department of ChemistrySchool of ScienceTianjin UniversityTianjin 300072China Collaborative Innovation Center of Chemical Science and Engineering Tianjin 300072China Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China Collaborative Innovation Center of Quantum Matter Beijing 100190China School of Physical Sciences University of Chinese Academy of SciencesBeijing 100049China Institute for New Energy Materials and Low-Carbon Technologies School of Materials Science and EngineeringTianjin Key Laboratory of Advanced Functional Porous MaterialsTianjin University of TechnologyTianjin 300384China

Rational design and synthesis of multimetallic nanostructures(NSs)are fundamentally important for electrochemical CO_(2)reduction reaction(CO_(2)RR).Herein,a multi-step seed-mediated growth method is applied to synthesize asymmetric AuAgCu heterostructures using Au nanobipyramids as nucleation seeds,in which their composition and structures are well *** find that the selectivity of C_(2)products for CO_(2)RR could be effectively regulated by tandem catalysis and electronic effect over trimetallic AuAgCu ***,the Faraday efficiency toward ethanol could reach up to 37.5%at a potential of−0.8 V versus reversible hydrogen electrode over asymmetric Au1Ag1Cu5 heterostructures with segregated domains of three constituent *** work provides an efficient strategy for the synthesis of multicomponent architectures to boost their promising application in CO_(2)RR.

关键词： CO_(2)reduction electrocatalysis tandem catalysis multimetallic nanostructure asymmetric heterostructure

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