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Factors Affecting the Catalytic Performance of Nano-catalysts

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Chinese Journal of Chemistry 2022年第4期40卷 515-523页

作者： Hongling Yang Yue Wu Zewen Zhuang Yang Li Chen Chen Department of Chemistry Tsinghua UniversityBeijing 100084China

Comprehensive Summary Nano-catalysis plays a vital role in the industrially chemical *** increasingly severe energy crisis and environmental issues spur scientists to exploit novel nano-catalysts in diverse *** is essential to understand the fundamental physicochemical properties of nano-catalysts to develop efficient systems,whose design can be subsequently precisely tuned at the atomic *** this review,we summarize several key factors affecting the catalytic activity of nano-catalysts,including structure,composition,size,and interface,providing guidance for the atomic level control of high-efficient ***,we present a brief conclusion and some thoughts on nano-catalysis.

关键词： heterogeneous catalysis Nano-catalysis Single-atom catalysis Structure-activity relationships Interfaces

SiO_(2)-Supported Ni(II)and Fe(II)Catalysts Bearing Sodium-Sulfonate Group for Olefin Polymerization

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Chinese Journal of Chemistry 2022年第23期40卷 2773-2779页

作者： Yao Sun Quan Wang Yao Pan Wenmin Pang Chen Zou Min Chen CAS Key Laboratory of Soft Matter Chemistry Department of Polymer Science and EngineeringUniversity of Science and Technology of ChinaHefeiAnhui 230026China Institutes of Physical Science and Information Technology Anhui UniversityHefeiAnhui 230601China

heterogeneous catalysts have been dominant for industrial polyolefin production,offering many distinct advantages,such as controlling the morphology of the polymer and preventing reactor *** this contribution,we designed several types of imine ligands bearing sodium-sulfonate ionic groups and the corresponding nickel/iron *** catalysts could be immobilized on SiO_(2)with strong affinity and high catalyst *** SiO_(2)-supported catalysts behaved better than their homogeneous counterparts during ethylene polymerization with extremely high activity(2.6×10^(4)kg·mol^(−1)·h^(−1))and high thermal *** addition,the supported nickel catalysts generated free-flowing polyethylene with high molecular weight(Mn up to 2.65×10^(3)kg·mol^(–1))and excellent morphology control,indicating no reactor fouling due to the leaching of ***,for copolymerization,immobilized nickel catalysts showed a higher tolerance of polar monomers,and the efficient copolymerization of ethylene with undecylenic acid was achieved with high activity(450 kg·mol^(−1)·h^(−1))and a high incorporation ratio(up to 12.3%).

关键词： heterogeneous catalysis Nickel iron catalysts Sodium-sulfonate group Polymerization Copolymerization

Recent advances in organic electrosynthesis using heterogeneous catalysts modified electrodes

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Chinese Chemical Letters 2023年第4期34卷 35-52页

作者： Li Ma Xianang Gao Xin Liu Xiaojun Gu Baoying Li Beibei Mao Zeyuan Sun Wei Gao Xiaofei Jia Jianbin Chen Shandong Provincial Key Laboratory of Molecular Engineering State Key Laboratory of Biobased Material and Green PapermakingSchool of Chemistry and Chemical EngineeringQilu University of Technology(Shandong Academy of Sciences)Ji’nan250353China College of Pharmacy Shandong University of Traditional Chinese MedicineJi’nan250355China Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science MOECollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China

Organic electrosynthesis as an emerging green and advantageous alternative to traditional synthetic methods has achieved remarkable progress in recent years because sustainable electricity can be employed as traceless redox agents. To surmount the over-oxidation/reduction issues of direct electrolysis,mediated or indirect electrochemical processes are attaining remarkable significance and promoting the selectivity of products. Molecular electrocatalysts, benefiting from the easily electronic and steric modulation, suffers from readily degradation issue in most cases. Remarkably, heterogeneous catalysts have drawn more attention due to their high activity, stability, and recyclability. Hence, in this review, the most recent growth of heterogeneous catalysts modified electrodes for organic electrosynthesis were summarized, highlighting structural optimization and electrochemical performance of these materials as well as reaction mechanism. Furthermore, key challenges and future directions in this area were also discussed.

关键词： Organic electrosynthesis Indirect electrosynthesis heterogeneous catalysis Hybrid materials Electrocatalysis

Acidic Electrocatalytic Semihydrogenation of Alkynols to Alkenols on Copper Phosphide at Industrial-Level Current Density

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Chinese Journal of Chemistry 2023年第24期41卷 3618-3624页

作者： Sanyin Yang Jun Bu Rui Bai Jin Lin Siying An Yafei Wu Ying Guo Jie Gao Jian Zhang School of Chemistry and Chemical Engineering Northwestern Polytechnical UniversityXi'anShaanxi710129 China State Key Laboratory of Solidification Processing School of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi'anShaanxi710072 China Interdisciplinary Research Center of Biology & catalysis School of Life SciencesNorthwestern Polytechnical UniversityXi'anShaanxi710072 China

Alkenols are important intermediates for the industrial manufacture of various commodities and fine *** present,alkenols are produced via thermocatalytic semihydrogenation of corresponding alkynols using precious metal Pd-based catalysts in pressurized hydrogen *** this work,we highlight an efficient electrocatalytic strategy for selectively reducing alkynols to alkenols under ambient *** 2-methyl-3-butyn-2-ol as a model alkynol,Cu3P nanoarrays anchored on Cu foam remarkably deliver an industrial-level partial current density of 0.79 A·cm^(-2) and a specific selectivity of 98%for 2-methyl-3-buten-2-ol in acidic *** a 40-runs stability test,Cu3P nanoarrays maintain 90%alkynol conversion and 90%alkenol *** in a large two-electrode flow electrolyser,the single-pass alkynol conversion and alkenol selectivity of Cu3P nanoarrays exceed 90%.Moreover,this selective electrocatalytic hydrogenation approach is broadly feasible for the production of various water-soluble *** analyses,theoretical simulation and electrochemical in-situ infrared investigations together reveal that exothermic alkynol hydrogenation,facile alkenol desorption and formation of active H on Cu3P surfaces account for the excellent electrocatalytic performance.

关键词： Alkynol Alkenol Cu_(3)P nanoarrays Electrocatalysis Semihydrogenation Mass spectrometry IR spectroscopy heterogeneous catalysis

CoCo-PBA/tetrabutylammonium bromide as highly efficient catalyst for CO_(2) and epoxides coupling reaction under mild conditions

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Chinese Chemical Letters 2022年第2期33卷 1081-1086页

作者： Munir Ullah Khan Saﬁr Ullah Khan Jiraya Kiriratnikom Shah Zareen Xinghong Zhang MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027China Hefei National Laboratory for Physical Science at the Microscale School of Life SciencesUniversity of Science and Technology of ChinaHefei 230027China National Synchrotron Radiation Laboratory Department of Chemical Physics and Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education InstitutesUniversity of Science and Technology of ChinaHefei 230029China

The development of effective and low-energy-consumption catalysts for CO_(2)conversion into high-value-added products by constructing versatile active sites on the surface of heterogeneous compounds is an ur-gent and challenging *** this study,a stable and well-defined heterogeneous cobalt hexacyanocobal-tate(Co_(3)[Co(CN)_(6)]_(2)),typical cobalt Prussian blue analogue(CoCo-PBA)modified with tetrabutylammo-nium bromide(TBAB),is proven to be the superior catalyst for CO_(2)and epoxide coupling to produce cyclic carbonates with>99%yield under mild reaction conditions(1.0 MPa,65℃).Based on a series of characterizations,it is revealed that the CoCo-PBA structure can maintain relatively high thermal and chemical *** experiments exhibited that the CoCo-PBA system could retain 98%of the original activity after six reaction *** CoCo-PBA/TBAB catalytic system was also highly active for coupling CO_(2)with other industrial-grade *** results show the Co Co-PBA catalytic system potential flexibility and the generality of the catalyst preparation strategy.

关键词： CO_(2)conversion Cyclic carbonates Prussian blue analogue heterogeneous catalysis Co_(3)[Co(CN)_(6)]_(2)

Plasmonic Core-Shell Nanostructures Enhanced Spectroscopies

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Chinese Journal of Chemistry 2022年第3期40卷 392-406页

作者： Jun Zhou Di-Ye Wei Yu-Jin Zhang Hua Zhang Jian-Feng Li State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringCollege of MaterialsCollege of EnergyFujian Key Laboratory of Advanced MaterialsXiamen UniversityXiamenFujian 361005China College of Optical and Electronic Technology China Jiliong UniversityHangzhouZhejiang 310018China

Core-shell nanostructures constituted by a plasmonic core and an ultrathin shell have drawn enormous attentions in enhanced spectroscopies,catalysis,energy,and other fields because of their splendid properties such as multifunctionality,stability,and *** this article,we summarized the endeavors made by our group in the past decade about the core-shell nanostructures in the shell-isolated nanoparticle-enhanced Raman spectroscopy(SHINERS)and plasmon-enhanced ***,the potential challenges and perspectives about core-shell nanostructures in spectroscopies have also been ***,we believe this article would provide an avenue for a comprehensive understanding of enhanced spectroscopies with core-shell nanostructures.

关键词： Raman spectroscopy Nanostructures Electrochemistry heterogeneous catalysis In-situ characterization

Promoting Electrocatalytic CO_(2) Reduction to CO via Sulfur-Doped Co-N-C Single-Atom Catalyst

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Chinese Journal of Chemistry 2023年第24期41卷 3553-3559页

作者： Zhiming Wei Yuhang Liu Jie Ding Qinye He Qiao Zhang Yueming Zhai The Institute for Advanced Studies Wuhan UniversityWuhanHubei430072 China School of Materials Science and Engineering Suzhou University of Science and TechnologySuzhouJiangsu215009 China

Electrocatalytic reduction of CO_(2) to fuels and chemicals possesses huge potential to alleviate current environmental *** doping in metal-nitrogen-carbon(M-N-C)single-atom catalysts(SACs)has been found to be capable to promote the electrocatalytic CO_(2) reduction reaction(CO_(2)RR).However,the origin of the enhanced activity is still ***,we report that sulfur-doped cobalt-nitrogen-carbon single-atom catalyst(Co1-SNC)exhibits superior CO_(2)RR performance compared to sulfur-free counterpart(Co1-NC).On the basis of in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS),kinetic isotope effect(KIE)and theoretical calculation,it is demonstrated that sulfur doping can promote water activation,elevate the d-band center of Co active site,and reduce the free energy of*COOH intermediate *** work deepens the understanding of the CO_(2)RR chemistry over heteroatom-doped SACs for designing efficient CO_(2)RR processes.

关键词： Electrocatalytic CO_(2)reduction Doping heterogeneous catalysis Single-atom catalysts ATR-SEIRAS

Facile Synthesis and High-Value Utilization of Ammonia

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Chinese Journal of Chemistry 2022年第8期40卷 953-964页

作者： Yu Luo Shijing Liang Xiuyun Wang Bingyu Lin Chongqi Chen Lilong Jiang National Engineering Research Center of Chemical Fertilizer Catalyst Fuzhou UniversityFuzhouFujian 350002China Qingyuan Innovation Laboratory QuanzhouFujian 362801China

Ammonia is a key component in fertilizer and the carbon-free hydrogen *** ammonia synthesis and utilization have played a central role in the development of chemical *** industrial production of ammonia remains dependent on the energy-and carbon-intensive Haber-Bosch process.A major effort has been devoted to developing robust and efficient catalysts,as well as alternative benign ***,we detail our endeavors that develop the ammonia synthesis and decomposition catalysts,and utilize the ammonia *** firstly discuss the catalysts for ammonia synthesis via dissociative and associative process,and the regulation of catalysts'***,we review the burgeoning electrocata-lytic nitrogen reduction process,focusing on the enhanced catalytic performances by the regulation of the catalysts and the ***,we provide a novel high-value utilization of ammonia to achieve the"zero-carbon"circular *** promising catalysts,reactors,and ammonia energy systems have been discussed in *** end this Account that offers future research directions and prospects of ammonia.

关键词： Nitrogen fixation Ammonia-to-hydrogen Carbon-free heterogeneous catalysis Supported catalysts

heterogeneousα-Diimine Nickel Catalysts with Improved Catalytic Performance in Ethylene Polymerization

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Chinese Journal of Chemistry 2023年第10期41卷 1155-1162页

作者： Zhanshan Ma Mengli Xu Ningning Zhu Chen Tan Changle Chen CAS Key Laboratory of Soft Matter Chemistry Department of Polymer Science and EngineeringUniversity of Science and Technology of ChinaHefeiAnhui 230026China Institutes of Physical Science and Information Technology Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationKey Laboratory of Environment-Friendly Polymeric Materials of Anhui ProvinceAnhui UniversityHefeiAnhui 230601China

Heterogenization can improve the thermal tolerance of olefin polymerization catalysts and result in good product morphology con-trol,which are two important parameters for industrial polyethylene *** this work,α-diimine nickel catalysts bearing-OH or-ONa anchoring groups were designed and *** anchoring groups can enable facile heterogenization of the cata-lysts on *** heterogeneous catalysts demonstrated enhanced thermal stabilities,along with high catalytic activity at 120℃(up to 5.5×10^(6)g·PE·mol·Ni^(-1)·h^(-1)).Furthermore,the heterogenization process results in the improvements of many other parame-ters,including polymer morphology control,catalytic activity(up to 1.9×10^(7)g·PE·mol·Ni^(-1)·h^(-1))and polyethylene molecular weight(Mn up to 2.3×10^(6)g·mol^(-1)).More importantly,the structure and properties of the polymer products can be controlled by catalyst structures,polymerization conditions and heterogenization to achieve good mechanical properties and elasticity.

关键词： Ethylene polymerization Mechanical properties Nickel Supported catalysts heterogeneous catalysis Polymerization Morphology