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Stable Cobalt–Zeolite Propane-Dehydrogenation Catalysts Enabled by Reaction-Driven Reconstruction

Angewandte Chemie 2025年

作者： Qiang Liu Yongbin Yao Junmeng Li Jingnan Wang Lili Chen Wenlin Li Yangyang Guo Siyu Yao Yongan Yang Xi Wang School of Chemical Engineering and Technology Collaborative Innovation Center of Chemical Science and Engineering Institute of Molecular Plus Department of Chemistry Tianjin University Tianjin 300072 P.R. China Key Laboratory of Luminescence and Optical Information Ministry of Education School of Physical Science and Engineering Beijing Jiaotong University Beijing 100044 P.R. China State Key Laboratory of Heavy Oil Processing China University of Petroleum Beijing 102249 P.R. China Institute of Molecular Engineering Plus College of Chemistry Fuzhou University Fuzhou 350108 P.R. China Key Laboratory of Photochemistry Institute of Chemistry Chinese Academy of Sciences Beijing 100190 P.R. China College of Chemistry and Chemical Engineering State Key Laboratory of Clean and Efficient Coal Utilization Taiyuan University of Technology Taiyuan 030024 P.R. China CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Mesoscience and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 P.R. China College of Chemical and Biological Engineering Zhejiang University Hangzhou 310027 P.R. China

Cobalt-based catalysts have emerged as promising substitutes for Pt- and Cr-based propane dehydrogenation (PDH) catalysts. However, controlling the distribution of Co species and achieving stable active centers remains challenging. Here, we report that reaction-driven reconstruction of metallic cobalt (Co 0 ) species within pure silica MFI zeolite (S-1) into CoO x clusters within silanol nests during PDH yields efficient and durable performance. Atomically dispersed CoO x clusters exhibit exceptional durability and high propylene space-time yield (STY), maintaining an ultrahigh propylene STY of 17.2 mmol C3H6 g cat −1 h −1 for over 260 h under industrially relevant conditions, surpassing previous cobalt-based PDH catalysts. Moreover, the catalyst operates stably at 520 °C for 170 h with near-equilibrium propane conversions. Comprehensive characterizations indicate the dynamic evolution process from the silanol nests effectively capturing and stabilizing Co 0 species within S-1 zeolite, thereby promoting the dynamic formation of CoO x clusters during the PDH process. We also demonstrate that stable Co─O active centers formed by this unique anchoring strategy improve catalyst stability by suppressing coke formation and promoting efficient propane dehydrogenation.

关键词： Cobalt-zeolite catalyst CoOx Reconstruction Propane dehydrogenation Reaction-driven Stable

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Ultrathin Two-Dimensional Porous Fullerene Membranes for Ultimate Organic Solvent Separation

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Angewandte Chemie 2024年第18期136卷

作者： Dr. Xiaofang Chen Yifang Mu Chunxin Jin Yayu Wei Jinlin Hao Prof. Huanting Wang Prof. Dr. Jürgen Caro Prof. Aisheng Huang State Key Laboratory of Molecular & Process Engineering Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular Engineering East China Normal University 500 Dongchuan Road Shanghai 200241 China Department of Chemical and Biological Engineering Monash University Clayton Victoria 3800 Australia Institute of Physical Chemistry and Electrochemistry Leibniz University Hanover Callinstrasse 3 A 30167 Hannover Deutschland

Two-dimensional (2D) materials with high chemical stability have attracted intensive interest in membrane design for the separation of organic solvents. As a novel 2D material, polymeric fullerenes (C 60 ) ∞ with distinctive properties are very promising for the development of innovative membranes. In this work, we report the construction of a 2D (C 60 ) ∞ nanosheet membrane for organic solvent separation. The pathways of the (C 60 ) ∞ nanosheet membrane are constructed by sub-1-nm lateral channels and nanoscale in-plane pores created by the depolymerization of the (C 60 ) ∞ nanosheets. Attributing to ordered and shortened transport pathways, the ultrathin porous (C 60 ) ∞ membrane is superior in organic solvent separation. The hexane, acetone, and methanol fluxes are up to 1146.3±53, 900.4±41, and 879.5±42 kg ⋅ m −2 ⋅ h −1 , respectively, which are up to 130 times higher than those of the state-of-the-art membranes with similar dye rejection. Our findings demonstrate the prospect of 2D (C 60 ) ∞ as a promising nanofiltration membrane in the separation of organic solvents from macromolecular compounds such as dyes, drugs, hormones, etc.

关键词： 2D materials 2D membrane polymeric fullerene (C60)∞ organic solvent separation fullerene

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Catalytic Enantioselective Synthesis of Planar Chiral Pillararenes via Asymmetric Sonogashira Coupling

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Angewandte Chemie 2024年第3期137卷

作者： Xiao-Hua Zhou Xin Zhang Yi-Ru Song Xue Li Lin-Tao Bao Dr. Wei-Tao Xu Dr. Xu-Qing Wang Prof. Dr. Hai-Bo Yang Prof. Dr. Wei Wang Shanghai Key Laboratory of Green Chemistry and Chemical Processes State Key Laboratory of Petroleum Molecular and Process Engineering School of Chemistry and Molecular Engineering East China Normal University 3663 N. Zhongshan Road Shanghai 200062 China Shanghai Center of Brain-inspired Intelligent Materials and Devices East China Normal University Shanghai 200241 China

As a novel type of macrocycles with attractive planar chirality, pillar[5]arenes have gained increasing research interest over the past decades, enabling their widespread applications in diverse fields such as porous materials, molecular machines, and chiral luminescence materials. However, the catalytic methodology towards the enantioselective synthesis of planar chiral pillar[5]arenes remains elusive. Here we report a novel method for the enantioselective synthesis of planar chiral pillar[5]arenes via asymmetric Sonogashira coupling, giving access to a wide range of highly functionalized planar chiral pillar[5]arenes, including both homo- and hetero-rimmed ones, with excellent enantioselectivities. Attractively, the resultant planar chiral pillar[5]arenes show great potential for widespread use in many areas such as chiral luminescent materials. This work not only enables the successful synthesis of planar chiral pillar[5]arenes with abundant structural and functional diversity as key building blocks for practical applications but also enriches the asymmetric cross-coupling methodologies in organic synthetic chemistry.

关键词： asymmetric catalysis macrocycles dynamic kinetic resolution chiral rotaxanes circularly polarized luminescence

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Effect of iron transformation on Acidithiobacillus ferrooxidans bio-leaching of clay vanadium residue

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Journal of Central South University 2019年第4期26卷 796-805页

作者： FENG Ya-li WANG Hong-jun LI Hao-ran CHEN Xi-pei DU Zhu-wei KANG Jin-xing School of Civil and Resource Engineering University of Science and Technology Beijing Key State Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of Sciences

The acid bio-leaching process of vanadium extraction from clay vanadium water-leached residue was studied and the effect of the performance of iron transformation was *** ferrooxidans affects the dissolution of vanadium through the catalytic effect on Fe^3+/Fe^2+couple and material *** passivation of iron settling correlates with ferrous ion content in bio-leaching *** medium containing *** and Fe(Ⅲ),the increment in Fe(Ⅱ)concentration leads to the formation of jarosite,generating a decline in vanadium extraction *** of cyclic voltammetry shows that Fe(Ⅱ)ion is apt to be oxidized and translated into precipitate by ***,which strongly adsorbed to the surface of the ***(Ⅲ)ion promotes the vanadium extraction due to its oxidizing *** *** to Fe(Ⅲ)medium elevates the reduction of low valence state vanadium and facilitates the exchange of substance between minerals and *** motivates 3.8%and 21.8%increments in recovery ratio and leaching rate of vanadium compared to the Fe(Ⅲ)exclusive use,***,Fe(Ⅱ)ion impacts vanadium extraction slightly in sterile medium but negatively influences vanadium leaching in the presence of bacteria.

关键词： iron ion cycle Acidithiobacillus ferrooxidans passivation cyclic valtammetry clay vanadium

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Carbon Dioxide Sequestration via Steelmaking Slag Carbonation in Alkali Solutions: Experimental Investigation and process Evaluation

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Acta Metallurgica Sinica(English Letters) 2018年第7期31卷 771-784页

作者： Chen-Ye Wang Wei-Jun Bao Zhan-Cheng Guo Hui-Quan Li State Key Laboratory of Advanced Metallurgy University of Science and Technology Beijing Key Laboratory of Green Process and Engineering National Engineering Laboratory for Hydrometallurgical Cleaner Production Technology Institute of Process EngineeringChinese Academy of Sciences

Carbon dioxide mineral sequestration with steelmaking slag is a promising method for reducing carbon dioxide in a large- scale setting. Existing calcium oxide or calcium hydroxide in steelmaking slag can be easily leached by water, and the formed calcium carbonate can be easily wrapped on the surface of unreacted steelmaking slag particles. Thus, further increase in the carbonation reaction rate can be prevented. Enhanced carbon dioxide mineral sequestration with steel- making slag in dilute alkali solution was analysed in this study through experiments and process evaluation. Operating conditions, namely alkali concentration, reaction temperature and time, and liquid-to-solid ratio, were initially investigated. Then, the material and energy balance of the entire process was calculated, and the net carbon dioxide sequestration efficiency at different reaction times was evaluated. Results showed that dilute alkali solution participated in slowing down the leaching of active calcium in the steelmaking slag and in significantly improving carbonation conversion rate. The highest carbonation conversion rate of approximately 50% can be obtained at the optimal conditions of 20 g/L alkali concentration, 2 mL/L liquid-to-solid ratio, and 70 ℃ reaction temperature. Carbonation reaction time significantly influences the net carbon dioxide sequestration efficiency. According to calculation, carbon dioxide emission of 52.6 kg/t- slag was avoided at a relatively long time of 120 min.

关键词： Steelmaking slag Dilute alkali solution COe mineral sequestration. process evaluation

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Electrochemiluminescence Enhancement and Passivation Mitigation in Carbon Nitride Semiconductors via an Integrated Ternary Heterostructure Strategy

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Small (Weinheim an der Bergstrasse, Germany) 2024年第26期20卷 e2310476页

作者： Chulei Zhao Chaoyun Ma Min Wang Wenjing Lai Chenglin Hong Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan School of Chemistry and Chemical Engineering Shihezi University Shihezi Xinjiang 832000 P. R. China. State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources Xinjiang University Urumqi Xinjiang 830017 P. R. China. Xinjiang Key Laboratory of Coal Clean Conversion & Chemical Engineering Process School of Chemical Engineering and Technology Xinjiang University Urumqi Xinjiang 830017 P. R. China.

In recent years, carbon nitride (CN) has attracted substantial attention in the field of electrochemiluminescence (ECL) applications, owing to its outstanding optical and electronic properties. However, the passivation of CN during the ECL process has contributed to reduced stability and poor repeatability. While some studies have tried to boost ECL performance by altering CN through doping and vacancies, effectively suppressing CN passivation at high potentials continues to be challenge. In this study, the built-in electric field and the Schottky barrier effect is used to expedite the transfer of electrons from CN to the molybdenum disulfide (MoS) conduction band. This transfer deterred excessive electron injection into the CN band, thus mitigating its electrochemical degradation. Moreover, by introducing nickel nanoparticles (Ni NPs) as catalytic active sites, it is facilitated that the decomposition of potassium persulfate (KSO), thereby enhancing both the stability and intensity of ECL emission. In the end, the application of ternary heterostructure as sensing platform for the cancer biomarker carcinoembryonic antigen (CEA) demonstrated high sensitivity. This research introduces a novel approach to overcome CN passivation, paving the way for more promising applications of CN in energy, environmental, and biosensing fields.

关键词： built‐in electric field carbon nitride electrochemiluminescence inhibition passivation

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Advances in Z-scheme and S-scheme heterojunctions for photocatalytic and photoelectrocatalytic H 2 O 2 production

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Chinese Chemical Letters 2025年

作者： Xibao Li Yiyang Wan Fang Deng Yingtang Zhou Pinghua Chen Fan Dong Jizhou Jiang National-Local Joint Engineering Research Center of Heavy Metal Pollutants Control and Resource Utilization Nanchang Hangkong University Nanchang 330063 China Zhejiang Key Laboratory of Petrochemical Environmental Pollution Control National Engineering Research Center for Marine Aquaculture Marine Science and Technology College Zhejiang Ocean University Zhoushan 316004 China Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China Chengdu 611731 China School of Materials Science and Engineering State Key Laboratory of Green and Efficient Development of Phosphorus Resources Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education Key Laboratory of Green Chemical Engineering Process of Ministry of Education Hubei Key Laboratory of Plasma Chemistry and Advanced Materials Novel Catalytic Materials of Hubei Engineering Research Center Wuhan Institute of Technology Wuhan 430205 China

Photocatalytic and photoelectrocatalytic H 2 O 2 production has been identified as a significant pathway within environmental pollution control, green energy, medical treatment, sterilization and disinfection. However, conventional single-material photocatalysts struggle to fulfill the stringent criteria of high efficiency, stability, cost-effectiveness, and responsiveness to visible light. The elevated recombination rates of photogenerated charge carriers, coupled with the suboptimal utilization of visible light, have collectively constrained the photocatalytic and photoelectrocatalytic H 2 O 2 production. Heterojunction catalysts for the production of H 2 O 2 has become a focal point of research. This review commences by elucidating the fundaments underlying the photocatalytic and photoelectrocatalytic H 2 O 2 production. Subsequently, it delineates the distinctive electron transfer mechanisms of Z-scheme and S-scheme heterojunctions, which exhibit enhanced efficiency in the photocatalytic and photoelectrocatalytic H 2 O 2 production, along with a summary of strategies for the improvement of photocatalyst and photoelectrocatalyst performance. Furthermore, this review also outlines the latest fabrication strategies, state-of-the-art in-situ characterization techniques, machine learning and density functional theory (DFT) simulations for Z-scheme or S-scheme catalysts for the photocatalytic and photoelectrocatalytic H 2 O 2 production, and briefly describes the multifunctional applications in H 2 O 2 production. Ultimately, the review contemplates the prospective developmental trajectories and application potential of these heterojunction configurations for the photocatalytic and photoelectrocatalytic H 2 O 2 production.

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Cooperation of Different Active Sites to Promote CO2Electroreduction to Multi-carbon Products at Ampere-Level

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Angewandte Chemie 2024年第15期136卷

作者： Dawei Zhou Prof. Dr. Chunjun Chen Yichi Zhang Min Wang Shitao Han Xue Dong Ting Yao Dr. Shuaiqiang Jia Prof. Dr. Mingyuan He Prof. Dr. Haihong Wu Prof. Dr. Buxing Han Shanghai Key Laboratory of Green Chemistry and Chemical Processes State Key Laboratory of Petroleum Molecular & Process Engineering School of Chemistry and Molecular Engineering East China Normal University Shanghai 200062 China State Key Laboratory of Petroleum Molecular and Process engineering SKLPMPE Sinopec research institute of petroleum processing Co. LTD. Beijing 100083 China East China Normal University Shanghai 200062 China Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Center for Excellence in Molecular Sciences Center for Carbon Neutral Chemistry Institute of Chemistry Chinese Academy of Sciences Zhongguancun North First Street 2 Beijing 100190 P. R. China

Electroreduction of CO 2 to C 2+ products provides a promising strategy for reaching the goal of carbon neutrality. However, achieving high selectivity of C 2+ products at high current density remains a challenge. In this work, we designed and prepared a multi-sites catalyst, in which Pd was atomically dispersed in Cu (Pd−Cu). It was found that the Pd−Cu catalyst had excellent performance for producing C 2+ products from CO 2 electroreduction. The Faradaic efficiency (FE) of C 2+ products could be maintained at approximately 80.8 %, even at a high current density of 0.8 A cm −2 for at least 20 hours. In addition, the FE of C 2+ products was above 70 % at 1.4 A cm −2 . Experiments and density functional theory (DFT) calculations revealed that the catalyst had three distinct catalytic sites. These three active sites allowed for efficient conversion of CO 2 , water dissociation, and CO conversion, ultimately leading to high yields of C 2+ products.

关键词： carbon dioxide C2+ products multi- sites catalyst electrolysis green chemistry

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Efficient Electrosynthesis of Valuablepara-Benzoquinone from Aqueous Phenol on NiRu Hybrid Catalysts

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Angewandte Chemie 2024年第3期137卷

作者： Fuqiang Liu Wei Chen Prof. Tong Wang Juchao Zhang Deyong Yang Yinhao Dai Guizi Liu Prof. Jian Zhou Prof. Shuangyin Wang Prof. Xiaohong Guan Shanghai Engineering Research Center of Biotransformation of Organic Solid Waste School of Ecological and Environmental Sciences Institute of Eco-Chongming East China Normal University Shanghai 200241 China State Key Laboratory of Chemo/Bio-Sensing and Chemometrics College of Chemistry and Chemical Engineering Advanced Catalytic Engineering Research Center of the Ministry of Education Hunan University Changsha 410082 China State Key Laboratory of Molecular & Process Engineering Shanghai Engineering Research Center of Molecular Therapeutics and New Drug Development Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular Engineering East China Normal University Shanghai 200241 China

Electrocatalytic oxidation of aqueous phenol to para -benzoquinone ( p -BQ) offers a sustainable approach for both pollutant abatement and value-added chemicals production. However, achieving high phenol conversion and p -BQ yield under neutral conditions remains challenging. Herein, we report a Ni(OH) 2 -supported Ru nanoparticles (NiRu) hybrid electrocatalyst, which exhibits a superior phenol conversion of 96.5 % and an excellent p -BQ yield of 83.4 % at pH 7.0, significantly outperforming previously reported electrocatalysts. This exceptional performance benefits from the triple synergistic modulation of the NiRu catalyst, including enhanced phenol adsorption, increased p -BQ desorption, and suppressed oxygen evolution. By coupling a flow electrolyzer with an extraction-distillation separation unit, the simultaneous phenol removal and p -BQ recovery are realized. Additionally, the developed electrocatalytic system with the NiRu/C anode displays good stability, favorable energy consumption, and reduced greenhouse gas emissions for phenol-containing wastewater treatment, demonstrating its potential for practical applications. This work offers a promising strategy for achieving low-carbon emissions in phenol wastewater treatment.

关键词： phenol wastewater resource recovery para-benzoquinone electrosynthesis Ni-based catalysts

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Correction to: Body centered non-fullerene acceptors substitution on triangular shaped Sub-phthalocyanines (SubPcs) based A-D-A organic solar cells: A step toward new strategies for better performances

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Optical and Quantum Electronics 2021年第1期54卷 1-3页

作者： Abbas, Faheem Ali, Usman Ahmad, Hafiz Muhammad Rizwan Tallat, Aqsa Shehzad, Aamir Zeb, Zonish Hussain, Iqbal Saeed, Aamir Key Lab of Organic Optoelectronics and Molecular Engineering of Ministry of Education Department of Chemistry Tsinghua University Beijing People’s Republic of China Department of Chemistry University of Agriculture Faisalabad Pakistan Institute of Chemistry Beijing National Laboratories for Molecular Sciences Key Laboratories of Organic Solids Chinese Academy of Sciences Beijing People’s Republic of China University of Chinese Academy of Sciences Beijing People’s Republic of China Center for Advancing Materials Performance From the Nanoscale State Key Laboratory for Mechanical Behavior of Materials Xi’an Jiaotong University Xi’an People’s Republic of China Department of Physics International Islamic University Islamabad Pakistan State Key Laboratory for Structural Chemistry of Unstable and Stable Species Institute of Chemistry Chinese Academy of Sciences Beijing People’s Republic of China Key Laboratory of Green Process and Engineering Institute of Process Engineering Beijing Key Laboratories of Ionic Liquids Clean Process Chinese Academy of Sciences Beijing People’s Republic of China

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