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Elucidating Confinement and Microenvironment of Ru Clusters Stably Confined in MFI Zeolite for Efficient Propane Oxidation

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Angewandte Chemie 2024年第5期137卷

作者： Jingjing Wang Dr. Zeyu Jiang Hengyue Xu Prof. Xinzhe Li Dr. Yanfei Jian Dr. Lianghui Xia Dr. Pei Su Qiyuan Liu Prof. Shouning Chai Dr. Mudi Ma Dr. Abdallah Amedlous Dr. Mathias Barreau Prof. Zhengping Hao Prof. Jiaguo Yu Prof. Chi He State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an 710049 Shaanxi P.R. China Laboratoire Catalyse & Spectrochimie Normandie Univ ENSICAEN UNICAEN CNRS Caen 14000 France Department of Chemistry Tsinghua University Beijing 100084 P.R. China College of Environmental and Chemical Engineering Yanshan University Qinhuangdao 066004 P.R. China National Engineering Laboratory for VOCs Pollution Control Material & Technology University of Chinese Academy of Sciences Beijing 101408 P.R. China Laboratory of Solar Fuel Faculty of Materials Science and Chemistry China University of Geosciences Wuhan 430078 P.R. China

Achieving active and stable heterogeneous catalysts by encapsulating noble metal species within zeolites is highly promising for high utilization and cost efficiency in thermal and environmental catalytic reactions. Ru, considered an economical noble metal alternative with comparable performance, faces great challenges within MFI-type microporous zeolites due to its high cohesive energy and mobility. Herein, an innovative strategy was explored that couples hydrothermal in situ ligand protection with stepwise calcination in a flowing atmosphere to embed ultrasmall Ru clusters anchored at K + -healed silanol sites (≡Si−Ru δ+ −O−K complexes) within 10-membered ring sinusoidal channels of MFI. Comprehensive experiments and theoretical calculations unveiled that the interplay between confined Ru clusters and MFI induces local strain in MFI, creating a unique catalytic microenvironment around the Ru clusters. This synergy interaction enhances alkane deep oxidation as the confined Ru clusters and the MFI microenvironment collectively pre-activate C 3 H 8 and O 2 , facilitate the cleavage of C−H and C−C bonds at low temperatures. Notably, the stable geometric and electronic properties of the confined Ru show exceptional thermal stability up to 1000 °C, rivaling fresh catalysts. These findings shed vital methodological and mechanistic insights for developing efficacious heterogeneous catalysts for thermal catalysis.

关键词： heterogeneous catalysis microenvironment Ruthenium strain zeolite

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Modulating the Electronic Metal-Support Interactions in Single-Atom Pt1−CuO Catalyst for Boosting Acetone Oxidation

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Angewandte Chemie 2022年第28期134卷

作者： Dr. Zeyu Jiang Dr. Mingjiao Tian Dr. Meizan Jing Prof. Shouning Chai Dr. Yanfei Jian Dr. Changwei Chen Prof. Mark Douthwaite Dr. Lirong Zheng Dr. Mudi Ma Prof. Weiyu Song Prof. Jian Liu Prof. Jiaguo Yu Prof. Chi He State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an 710049 Shaanxi P. R. China Department of Chemistry National University of Singapore Singapore 117543 Singapore Laboratory of Solar Fuel Faculty of Materials Science and Chemistry China University of Geosciences Wuhan 430074 P. R. China State Key Laboratory of Heavy Oil Processing China University of Petroleum Beijing 102249 P. R. China Max Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis School of Chemistry Cardiff University Cardiff CF10 3AT UK Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 P. R. China National Engineering Laboratory for VOCs Pollution Control Material & Technology University of Chinese Academy of Sciences Beijing 101408 P. R. China

The development of highly active single-atom catalysts (SACs) and identifying their intrinsic active sites in oxidizing industrial hazardous hydrocarbons are challenging prospects. Tuning the electronic metal-support interactions (EMSIs) is valid for modulating the catalytic performance of SACs. We propose that the modulation of the EMSIs in a Pt 1 −CuO SAC significantly promotes the activity of the catalyst in acetone oxidation. The EMSIs promote charge redistribution through the unified Pt−O−Cu moieties, which modulates the d -band structure of atomic Pt sites, and strengthens the adsorption and activation of reactants. The positively charged Pt atoms are superior for activating acetone at low temperatures, and the stretched Cu−O bonds facilitate the activation of lattice oxygen atoms to participate in subsequent oxidation. We believe that this work will guide researchers to engineer efficient SACs for application in hydrocarbon oxidation reactions.

关键词： Acetone Oxidation Electronic Metal-Support Interactions Intrinsic Mechanism Single-Atom Catalysts

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Calcined [email protected] @Rh x Ni 1- x : A novel hierarchically oriented composition tunable catalyst for green and sustainable hydrogen generation

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Journal of Environmental Chemical engineering 2022年第3期10卷

作者： Yasir Abbas Zareen Zuhra Sahresh Majeed Muhammad Shuaib Khan Majid Basharat Deependra Tyagi Shafqat Ali Zhanpeng Wu Zhaojun Liu Department of Electrical and Electronic Engineering Southern University of Science and Technology 1088 Xueyuan Blvd Nanshan District Shenzhen 518055 PR China State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical Technology Beijing 100029 PR China Department of Environment and Civil Engineering Dongguan University of Technology Dongguan 523808 PR China Institute of Chemical Sciences Bahauddin Zakariya University Multan 60800 Pakistan International Research Center for Renewable Energy (IRCRE) State Key Laboratory of Multiphase Flow in Power Engineering (MPFE) Xi’an Jiaotong University Xi’an 710049 PR China Institute for Advanced Study Shenzhen University Nanhai Avenue 3688 Shenzhen 518060 PR China

The ever decreasing amount of fossil fuels and increasing environmental pollution are alarming threats for green and sustainable future. Designing a new catalyst is, therefore, of paramount significance in the quest to discover sustainable, robust, and environmentally benign materials for clean and sustainable energy generation. Herein, we developed a hierarchically oriented catalyst of calcined poly(ferrocenedimethano)-cyclotriphosphazene-microspheres (CPFC-MS) supported with nickel-aluminum layered double hydroxide and decorated with nanoparticles (NPs) of rhodium-nickel, [email protected] x Ni 1 - x ( x = 2.06–6.75), for H 2 generation from ammonia borane (AB) hydrolysis . The highly active catalyst was characterized by scanning electron microscopy (SEM), Raman spectroscopy , high-resolution transmission electron microscopy (HRTEM) and TEM, energy dispersive X-ray spectroscopy (EDX), fourier transform infrared (FTIR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS). The as-fabricated [email protected] @Rh x Ni 1- x ( x = 2.06–6.75) catalysts were tested for AB hydrolysis and the results showed remarkable performance and higher stability for H 2 generation. The [email protected] @Rh 2.06 Ni 7.32 catalyst, having the lowest Rh-contents, exhibited maximum H 2 generation with a turn over frequency (TOF) of 780 mol H 2 hr −1 mol Rh −1 and an activation energy (E a ) of 40.3 kJ/mol with excellent sustainability . The superior activity is ascribed to the synergetic effect between RhNi NPs and their well-dispersion over hierarchically oriented [email protected] support, while higher stability due to LDH-AlNi/RhNi attractions. This work will provide new opportunities for polyphosphazenes and LDH derived hierarchically oriented sustainable catalysts for green energy production for sustainable future.

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Exploration over combined impacts of modified piston bowl geometry and tert -butyl hydroquinone additive-included biodiesel/diesel blend on diesel engine behaviors

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Fuel 2022年 322卷

作者： Krupakaran Radhakrishnan Lawrence Zuohua Huang Xuan Phuong Nguyen Dhinesh Balasubramanian Vidyasagar Reddy Gangula Raghurami Reddy Doddipalli Van Vang Le Sachuthananthan Bharathy Anh Tuan Hoang Department of Mechanical Engineering Sree Vidyanikethan Engineering College Tirupati Andhra Pradesh India State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi’an 710049 China PATET Research Group Ho Chi Minh City University of Transport Ho Chi Minh City Viet Nam Department of Mechanical Engineering Mepco Schlenk Engineering College Sivakasi India Mechanical Engineering Faculty of Engineering Khon Kaen University Khon Kaen Thailand Center for Alternative Energy Research and Development Khon Kaen University Khon Kaen Thailand Institute of Maritime Ho Chi Minh City University of Transport Ho Chi Minh City Viet Nam Institute of Engineering HUTECH University Ho Chi Minh City Viet Nam

Nowadays, the use of biodiesel for diesel engines has been attracting researchers aiming to improve engine characteristics although the engine performance could be decreased while utilizing biodiesel. In this aspect, optimizing the piston bowl geometry is one of the useful approaches to enhance the efficiency of the biodiesel-powered diesel engine. In this study, the standard piston of an existing diesel engine was modified into two different combustion bowls, namely Symmetrical Stepped Curved-V (SSCV) and Symmetrical Spline-V (SSV), to evaluate the CI engine performance powered with mixtures of sesame-originated biodiesel, diesel fuel, and tert -butyl hydroquinone (TBHQ) additive through two-stage experiment. In the first phase, experiments were carried out on two modified piston bowls powered by diesel and S20 (20% sesame biodiesel + 80% diesel fuel). Resultantly, SSV piston revealed superior engine characteristics to SSCV piston and standard piston due to enhanced air–fuel mixing and more complete combustion of SSV piston-based engine. Indeed, SSV piston operation exhibited an 8.68% of increased brake thermal efficiency (BTE), 6.54% of curtailed brake-specific fuel consumption (BSFC), 4.76% of lowered carbon monoxide (CO), 4.84% of decreased unburnt hydrocarbon (HC), and 2.22% of lowered smoke opacity but with increased nitrogen oxide (NOx) by 14.14% in comparison to diesel. In the 2nd phase, to control the NOx emission effectively, a TBHQ additive was added to the S20 sample at different proportions (500 mg and 1000 mg) to analyze the test engine behaviors with modified piston shapes. As a result, S20 + 500 mg TBHQ at 100% load improved BTE by 5.79% and reduced BSFC by 4.36% in the case of SSV piston. Moreover, it curtailed emissions of CO, HC, NOx, and smoke opacity by 13.33%, 15.49%, 12.09%, and 9.44%, respectively, when equated with diesel. Overall, S20 + 500 mg TBHQ could be thought of as a possible alternative fuel on SSV piston as it resulted in superior p

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Room‐Temperature Activation of H2by a Surface Frustrated Lewis Pair

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Angewandte Chemie 2019年第28期131卷

作者： Lu Wang Tingjiang Yan Rui Song Wei Sun Yuchan Dong Jiuli Guo Zizhong Zhang Xuxu Wang Geoffrey A. Ozin Department of Chemistry University of Toronto 80 St. George Street Toronto Ontario M5S3H6 Canada College of Chemistry and Chemical Engineering Qufu Normal University Qufu Shandong 273165 P. R. China International Research Center for Renewable Energy & State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an Shanxi 710049 P. R. China Department of Chemistry Nankai University Tianjin 300071 P. R. China State Key Laboratory of Photocatalysis on Energy and Environment College of Chemistry Fuzhou University Fuzhou 350108 P. R. China

Surface frustrated Lewis pairs (SFLPs) have been implicated in the gas‐phase heterogeneous (photo)catalytic hydrogenation of CO 2 to CO and CH 3 OH by In 2 O 3− x (OH) y . A key step in the reaction pathway is envisioned to be the heterolysis of H 2 on a proximal Lewis acid–Lewis base pair, the SFLP, the chemistry of which is described as In⋅⋅⋅In‐OH + H 2 → In‐OH 2 + ⋅⋅⋅In‐H − . The product of the heterolysis, thought to be a protonated hydroxide Lewis base In‐OH 2 + and a hydride coordinated Lewis acid In‐H − , can react with CO 2 to form either CO or CH 3 OH. While the experimental and theoretical evidence is compelling for heterolysis of H 2 on the SFLP, all conclusions derive from indirect proof, and direct observation remains lacking. Unexpectedly, we have discovered rhombohedral In 2 O 3− x (OH) y can enable dissociation of H 2 at room temperature, which allows its direct observation by several analytical techniques. The collected analytical results lean towards the heterolysis rather than the homolysis reaction pathway.

关键词： Gasphasenreaktionen Heterolytische H2-Dissoziation Indiumoxid Oberflächenchemie Oberflächenfrustriertes Lewis-Paar

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Corrigendum to: “One-pot synthesis of amorphous/crystalline SnO 2 /BaSO 4 composite sensitized with Eosin Y for enhanced photocatalytic H 2 production” [J. Environ. Chem. Eng. 12 (2024) 112770/JECE112770]

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Journal of Environmental Chemical engineering 2024年第5期12卷

作者： Cheng Cheng Jinfeng Zhang Haiping Jia Xutao Ding Gongyue Dong Feng Chen Yuchao Hu Jinwen Shi School of Chemical Engineering and Technology International Research Center for Renewable Energy (IRCRE) State Key Laboratory of Multiphase Flow in Power Engineering (MFPE) Xi’an Jiaotong University (XJTU) 28 West Xianning Road Xi’an 710049 China Shaanxi Key Laboratory of Advanced Stimulation Technology for Oil & Gas Reservoirs Xi’an Shiyou University Xi’an 710065 China Shaanxi Gas Group Fuping Energy Technology Co. Ltd 2 Kaiyuan Road Xi'an 710016 China Integrated Energy Institute Sichuan Digital Economy Industry Development Research Institute 88 Jiefang Road Chengdu 610036 China West Pipeline Company PipeChina 666 Beijing Middle Road Urumqi 830013 China School of Materials and Energy University of Electronic Science and Technology of China Chengdu 611731 China

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A ‐Oriented Hittorf's Phosphorus Nanorods/Polymeric Carbon Nitride Heterostructure for Boosting Wide‐Spectrum‐Responsive Photocatalytic Hydrogen Evolution from Pure Water

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Angewandte Chemie 2019年第2期132卷

作者： Yukun Zhu Chunxiao Lv Zhuocheng Yin Jun Ren Xianfeng Yang Chung‐Li Dong Hongwei Liu Rongsheng Cai Yu‐Cheng Huang Wolfgang Theis Shaohua Shen Dongjiang Yang State Key Laboratory of Bio-fibers and Eco-textiles Shandong Collaborative Innovation Center of Marine Biobased Fibers and Ecological Textiles Institute of Marine Biobased Materials School of Environmental Science and Engineering Qingdao University Qingdao 266071 P. R. China International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an 710049 P. R. China School of Chemical and Environmental Engineering North University of China Taiyuan 030051 P. R. China Analytical and Testing Centre South China University of Technology Guangzhou 510640 P. R. China Research Center for X-ray Science & Department of Physics Tamkang University Tamsui 25137 Taiwan The Australian Centre for Microscopy & Microanalysis The University of Sydney Sydney New South Wales 2006 Australia Nanoscale Physics Research Laboratory School of Physics and Astronomy University of Birmingham Birmingham B15 2TT UK

Red phosphorus is a promising photocatalyst with wide visible‐light absorption up to 700 nm, but the fast charge recombination limits its photocatalytic hydrogen evolution reaction (HER) activity. Now, [001]‐oriented Hittorf's phosphorus (HP) nanorods were successfully grown on polymeric carbon nitride (PCN) by a chemical vapor deposition strategy. Compared with the bare PCN and HP, the optimized PCN@HP hybrid exhibited a significantly enhanced photocatalytic activity, with HER rates reaching 33.2 and 17.5 μmol h −1 from pure water under simulated solar light and visible light irradiation, respectively. It was theoretically and experimentally indicated that the strong electronic coupling between PCN and [001]‐oriented HP nanorods gave rise to the enhanced visible light absorption and the greatly accelerated photoinduced electron–hole separation and transfer, which benefited the photocatalytic HER performance.

关键词： Heterostrukturen Nanostäbe Hittorfscher Phosphor Kohlenstoffnitrid Wasserspaltung

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Solar Hydrocarbons: Single-Step, Atmospheric-Pressure Synthesis of C2−C4Alkanes and Alkenes from CO2

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Angewandte Chemie 2023年第27期135卷

作者： Rui Song Zhao Li Jiuli Guo Paul N. Duchesne Chenyue Qiu Chengliang Mao Jia Jia Sanli Tang Yang-Fan Xu Wenzhe Zhou Lu Wang Wei Sun Xiaoliang Yan Liejin Guo Dengwei Jing Geoffrey A. Ozin International Research Center for Renewable Energy & State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an Shaanxi 710049 China Solar Fuels Group Department of Chemistry University of Toronto 80 St. George Street Toronto Ontario M5S 3H6 Canada Contribution: Conceptualization (equal) Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Writing - original draft (equal) Contribution: Data curation (supporting) Formal analysis (equal) Writing - original draft (supporting) School of Chemistry and Chemical Engineering Anyang Normal University Anyang Henan 455000 P. R. China Contribution: Data curation (supporting) Formal analysis (supporting) Methodology (equal) Software (supporting) Writing - original draft (supporting) Contribution: Data curation (supporting) Software (lead) Department of Materials Science and Engineering University of Toronto Toronto Ontario M5S 3E4 Canada Contribution: Data curation (supporting) Contribution: Conceptualization (supporting) Contribution: Formal analysis (supporting) Contribution: Methodology (supporting) State Key Laboratory of Silicon Materials and School of Materials Science and Engineering Zhejiang University Hangzhou Zhejiang 310058 China Contribution: Project administration (supporting) Contribution: Conceptualization (lead) Formal analysis (lead) Funding acquisition (equal) Project administration (equal) Supervision (equal) Writing - original draft (lead) Contribution: Conceptualization (lead) Funding acquisition (equal) Project administration (equal) Writing - original draft (lead)

Cobalt ferrite (CoFe 2 O 4 ) spinel has been found to produce C 2 −C 4 hydrocarbons in a single-step, ambient-pressure, photocatalytic hydrogenation of CO 2 with a rate of 1.1 mmol g −1 h −1 , selectivity of 29.8 % and conversion yield of 12.9 %. On stream the CoFe 2 O 4 reconstructs to a CoFe−CoFe 2 O 4 alloy-spinel nanocomposite which facilitates the light-assisted transformation of CO 2 to CO and hydrogenation of the CO to C 2 −C 4 hydrocarbons. Promising results obtained from a laboratory demonstrator bode well for the development of a solar hydrocarbon pilot refinery.

关键词： C2−C4 Hydrocarbons CO2 Hydrogenation Cobalt Ferrite Photocatalysis

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