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Photothermal Synergistic Effect Induces Bimetallic Cooperation to Modulate Product Selectivity of CO2Reduction on Different CeO2Crystal Facets

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Angewandte Chemie 2024年第46期136卷

作者： Yuqi Ren Yitao Si Mingyue Du Changjun You Chunyang Zhang Yuan-Hao Zhu Prof. Zhenkun Sun Prof. Kai Huang Prof. Maochang Liu Prof. Lunbo Duan Prof. Naixu Li School of Chemistry and Chemical Engineering Southeast University No.2 Dongnandaxue Road Nanjing 211189 Jiangsu P.R. China International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University No.28 Xianning West Road Xi'an Shaanxi 710049 P.R. China Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education School of Energy and Environment No.2 Dongnandaxue Road Nanjing 210096 Jiangsu P.R. China

Product selectivity of solar-driven CO 2 reduction and H 2 O oxidation reactions has been successfully controlled by tuning the spatial distance between Pt/Au bimetallic active sites on different crystal facets of CeO 2 catalysts. The replacement depth of Ce atoms by monatomic Pt determines the distance between bimetallic sites, while Au clusters are deposited on the surface. This space configuration creates a favourable microenvironment for the migration of active hydrogen species (*H). The *H is generated via the activation of H 2 O on monatomic Pt sites and migrate towards Au clusters with a strong capacity for CO 2 adsorption. Under concentrated solar irradiation, selectivity of the (100) facet towards CO is 100 %, and the selectivity of the (110) and (111) facets towards CH 4 is 33.5 % and 97.6 %, respectively. Notably, the CH 4 yield on the (111) facet is as high as 369.4 μmol/g/h, and the solar-to-chemical energy efficiency of 0.23 % is 33.8 times higher than that under non-concentrated solar irradiation. The impacts of high-density flux photon and thermal effects on carriers and *H migration at the microscale are comprehensively discussed. This study provides a new avenue for tuning the spatial distance between active sites to achieve optimal product selectivity.

关键词： Photothermal catalysis CO2 reduction Product selectivity Bimetallic active sites Spatial distance

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Sodium-Ion Batteries: Carbon-Based Alloy-Type Composite Anode Materials toward Sodium-Ion Batteries (Small 22/2019)

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Small 2019年第22期15卷

作者： Guorui Yang P. Robert Ilango Silan Wang Muhammad Salman Nasir Linlin Li Dongxiao Ji Yuxiang Hu Seeram Ramakrishna Wei Yan Shengjie Peng Department of Chemistry School of Science Xi'an Jiaotong University Xi'an 710049 P. R. China Department of Environmental Science & Engineering State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an 710049 China Department of Mechanical Engineering National University of Singapore Singapore 117574 Singapore Jiangsu Key Laboratory of Electrochemical Energy Storage Technologies College of Materials Science and Technology Nanjing University of Aeronautics and Astronautics Nanjing 210016 China Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Nankai University Tianjin 300071 China Nanomaterials Centre School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnology The University of Queensland QLD 4072 Australia

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Interface engineering of Z-scheme heterojunction for photocatalytic water splitting

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Fundamental Research 2024年

作者： Daming Zhao Yuxiao Yang Vasileios Binas Shaohua Shen School of Advanced Energy Shenzhen Campus of Sun Yat-sen University Shenzhen 518107 China Institute of Electronic Structure and Laser (IESL) FORTH P.O. Box 1527 Vasilika Vouton GR-71110 Heraklion Greece Physical Chemistry Laboratory Chemistry Department Aristotle University of Thessaloniki 54124 Thessaloniki Greece International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an 710049 China

Photocatalytic water splitting technology can directly convert solar energy into H 2 via a zero-carbon route, offering a sustainable solution for solar utilization and H 2 supply. Among various developed photocatalysts, Z-scheme heterojunction mimicking natural photosynthesis by combining two dissimilar semiconductors for redox reactions in series has unequivocally demonstrated its superiority in enhanced charge transfer, robust redox driving force, and wide optical absorption range. A comprehensive understanding on the fundamental principles of interface engineering between semiconductor components is the key to construct an efficient Z-scheme heterojunction. By focusing on different types of semiconductors, this article thoroughly expounds the coupling principles of components in binary mediator-free and ternary solid-mediator Z-scheme heterojunctions for photocatalytic water splitting, from the viewpoint of band structure alignment and interfacial electric field design. In addition to the well summarized research progresses in recent years, perspectives on the challenges and opportunities for developing advanced Z-scheme heterojunctions are provided.

关键词： Interface engineering Z-scheme heterojunction Water splitting Photocatalysis Solar energy conversion

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Excess thermodynamic properties and FTIR studies of binary of 1, 3-dichlorobenzene with alkyl acetates (C1–C5) at different temperatures

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Chemical Data Collections 2020年 29卷

作者： R. Raju S. Ravikumar R. Gerald Arokiaraj S. Karlapudi K. Sivakumar V. Pandiyan Department of Physics Nehru Memorial College (Autonoums) Puthanampatti 621 007Tamil Nadu India. State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Shaanxi 710049 P. R. China. Department of Chemistry S.V.Arts Degree & P.G.College (T.T.D'S) Tirupati 517502 A.P India

Densities ( ρ ) and speed of sound ( u ) have been reported for the binary mixtures containing 1, 3- dichlorobenzene (1, 3-DCB) with methyl acetate, ethyl acetate, propyl acetate, butyl acetate and pentyl acetate at four different temperatures ( T = 303.15, 308.15, 313.15 and 318.15 K) and at atmospheric pressure. The experimental data of densities and speeds of sound has been further utilized to calculate excess molar volume ( V m E ) and excess isentropic compressibility ( κ S E ) the excess properties have been fitted to Redlich-Kister equation. Further, V m E results have also been discussed by using Prigogine–Flory–Patterson (PFP). The experimental speeds of sound data in the present investigated mixtures were compared with various theoretical models like collision factor theory (CFT) and free length theory (FLT) to check their relative merits of pure component properties. Moreover, the experimental excess functions were correlated in terms of FTIR spectral analysis.

关键词： Binary mixtures Densities Ester Halogenated benzene Speed of sound FTIR

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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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Decrypting the Controlled Product Selectivity over Ag−Cu Bimetallic Surface Alloys for Electrochemical CO2Reduction

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Angewandte Chemie 2023年第19期135卷

作者： Daixing Wei Yiqing Wang Prof. Chung-Li Dong Zhengqi Zhang Xinyu Wang Dr. Yu-Cheng Huang Yuchuan Shi Xiaoli Zhao Jialin Wang Prof. Ran Long Prof. Yujie Xiong Prof. Fan Dong Prof. Mingtao Li Prof. Shaohua Shen International Research Center for Renewable Energy State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Xi'an 710049 China Department of Physics Tamkang University New Taipei City 25137 Taiwan Hefei National Laboratory for Physical Sciences at the Microscale Frontiers Science Center for Planetary Exploration and Emerging Technologies School of Chemistry and Materials Science and National Synchrotron Radiation Laboratory University of Science and Technology of China Hefei 230026 China Research Center for Environmental and Energy Catalysis Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China Chengdu 611731 China

Electrochemical CO 2 reduction reaction (ECO 2 RR) with controlled product selectivity is realized on Ag−Cu bimetallic surface alloys, with high selectivity towards C2 hydrocarbons/alcohols (≈60 % faradaic efficiency, FE), C1 hydrocarbons/alcohols (≈41 % FE) and CO (≈74 % FE) achieved by tuning surface compositions and applied potentials. In situ spectral investigations and theoretical calculations reveal that surface-composition-dependent d-band center could tune *CO binding strengths, regulating the *CO subsequent reaction pathways and then the product selectivity. Further adjusting the applied potentials will alter the energy of participated electrons, which leads to controlled ECO 2 RR selectivity towards desired products. A predominant region map, with an indicator proposed to evaluate the thermodynamic predominance of the *CO subsequent reactions, is then provided as a reliable theoretical guidance for the controllable ECO 2 RR product selectivity over bimetallic alloys.

关键词： Alloys CO2 Reduction Controlled Product Selectivity Electrochemistry

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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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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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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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