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Overturned Loading of Inert CeO2to Active Co3O4for Unusually Improved Catalytic Activity in Fenton-Like Reactions

Angewandte Chemie 2022年第16期134卷

作者： Chunli Song Qing Zhan Dr. Fei Liu Chuan Wang Dr. Hongchao Li Xuan Wang Prof. Xuefeng Guo Prof. Yingchun Cheng Wei Sun Prof. Li Wang Prof. Jieshu Qian Prof. Bingcai Pan Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse School of Environmental and Biological Engineering Nanjing University of Science and Technology 200 Xiao Ling Wei Nanjing 210094 China Key Laboratory of Flexible Electronics & Institute of Advanced Materials Jiangsu National Synergetic Innovation Center for Advanced Materials Nanjing Tech University Nanjing 211816 China Key Lab of Mesoscopic Chemistry MOE School of Chemistry & Chemical Engineering Nanjing University Nanjing 210023 China Key Laboratory of Catalysis and Energy Materials Chemistry of Ministry of Education South-Central University for Nationalities Wuhan 430074 China Research Center for Environmental Nanotechnology (ReCENT) School of Environment State Key Laboratory of Environmental Pollution and Resources Reuse Nanjing University Nanjing 210023 China

In the past decades, numerous efforts have been devoted to improving the catalytic activity of nanocomposites by either exposing more active sites or regulating the interaction between the support and nanoparticles while keeping the structure of the active sites unchanged. Here, we report the fabrication of a Co 3 O 4 −CeO 2 nanocomposite via overturning the loading direction, i.e., loading an inert CeO 2 support onto active Co 3 O 4 nanoparticles. The resultant catalyst exhibits unexpectedly higher activity and stability in peroxymonosulfate-based Fenton-like reactions than its analog prepared by the traditional impregnation method. Abundant oxygen vacancies (O v with a Co⋅⋅⋅O v ⋅⋅⋅Ce structure instead of Co⋅⋅⋅O v ) are generated as new active sites to facilitate the cleavage of the peroxide bond to produce SO 4 .− and accelerate the rate-limiting step, i.e., the desorption of SO 4 .− , affording improved activity. This strategy is a new direction for boosting the catalytic activity of nanocomposite catalysts in various scenarios, including environmental remediation and energy applications.

关键词： CO Oxidation Fenton-Like Reaction Nanocomposite Catalyst Overturned Loading Oxygen Vacancy

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Cancer Therapy: Dual Intratumoral Redox/Enzyme‐Responsive NO‐Releasing Nanomedicine for the Specific, High‐Efficacy, and Low‐Toxic Cancer Therapy (Adv. Mater. 30/2018)

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advanced Materials 2018年第30期30卷

作者： Xiaobo Jia Yihua Zhang Yu Zou Yao Wang Dechao Niu Qianjun He Zhangjian Huang Weihong Zhu He Tian Jianlin Shi Yongsheng Li Lab of Low‐Dimensional Materials Chemistry Key Laboratory for Ultrafine Materials of Ministry of Education School of Materials Science and Engineering East China University of Science and Technology Shanghai 200237 P. R. China State Key Laboratory of Natural Medicines Jiangsu Key Laboratory of Drug Discovery for Metabolic Diseases China Pharmaceutical University Nanjing 210009 P. R. China Guangdong Key Laboratory for Biomedical Measurements and Ultrasound Imaging School of Biomedical Engineering Health Science Center Shenzhen University Shenzhen 518060 China Shanghai Key Laboratory of Functional Materials Chemistry Key Laboratory for Advanced Materials and Institute of Fine Chemicals East China University of Science & Technology Shanghai 200237 China

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Cover Image, Volume 6, Number 3, March 2024

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Carbon Energy 2024年第3期6卷

作者： Xiaofei Zhang Wenhuan Huang Le Yu Max García-Melchor Dingsheng Wang Linjie Zhi Huabin Zhang KAUST Catalysis Center (KCC) King Abdullah University of Science and Technology (KAUST) Thuwal Saudi Arabia Key Laboratory of Chemical Additives for China National Light Industry College of Chemistry and Chemical Engineering Shaanxi University of Science and Technology Xi'an China Linjie Zhi Advanced Chemical Engineering and Energy Materials Research Center China University of Petroleum (East China) Qingdao 266580 China. State Key Lab of Organic-Inorganic Composites Beijing University of Chemical Technology Beijing China School of Chemistry CRANN and AMBER Research Centres Trinity College Dublin College Green Dublin Ireland Department of Chemistry Tsinghua University Beijing China Advanced Chemical Engineering and Energy Materials Research Center China University of Petroleum (East China) Qingdao China Wenhuan Huang Key Laboratory of Chemical Additives for China National Light Industry College of Chemistry and Chemical Engineering Shaanxi University of Science and Technology Xi'an 710021 China.

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Back Cover: Hexabenzoheptacene: A Longitudinally Multihelicene Nanocarbon with Local Aromaticity and Enhanced Stability (Angew. Chem. Int. Ed. 29/2024)

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Angewandte Chemie International Edition 2024年第29期63卷

作者： Xinyue Liu Zhengxiong Jin Fei Qiu Yupeng Guo Yan Chen Prof. Zhe Sun Prof. Lei Zhang Beijing Advanced Innovation Center for Soft Matter Science and Engineering State Key Lab of Organic-Inorganic Composites Beijing University of Chemical Technology Beijing 100029 P. R. China Institute of Molecular Plus Department of Chemistry and Haihe Laboratory of Sustainable Chemical Transformation Tianjin University 92 Weijin Road Tianjin 300072 P. R. China

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Hexabenzoheptacene: A Longitudinally Multihelicene Nanocarbon with Local Aromaticity and Enhanced Stability

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Angewandte Chemie 2024年第29期136卷

We report the synthesis of a longitudinally helical molecular nanocarbon, hexabenzoheptacene ( HBH ), along with its dimethylated derivative ( HBH-Me ), which are composed of six benzene rings periodically benzannulated to both zigzag edges of a heptacene core. This benzannulation pattern endows the resulting nanocarbons with a helical heptacene core and local aromaticity, imparting enhanced solubility and stability to the system. The chiral HBH-Me adopts a more highly twisted conformation with an end-to-end twist angle of 95°, enabling the separation of the enantiomers. Both HBH and HBH-Me can be facilely oxidized into their corresponding dications, which exhibit enhanced planarity and aromaticity upon loss of electrons. Notably, both longitudinally helical nanocarbons readily promote solid state packing into two-dimensional (2D) arrangement. Single-crystal microbelts of HBH-Me show hole mobility up to 0.62 cm 2 V −1 s −1 , illustrating the promising potential of these longitudinally helical molecules for organic electronic devices.

关键词： heptacene benzannulation nanocarbon helicene organic field-effect transistor

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Rücktitelbild: Hexabenzoheptacene: A Longitudinally Multihelicene Nanocarbon with Local Aromaticity and Enhanced Stability (Angew. Chem. 29/2024)

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Angewandte Chemie 2024年第29期136卷

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All-perovskite tandem 1 cm2 cells with improved interface quality

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Nature 2023年 80-86页

作者： Rui He Zongjin Yi Cong Chen Jincheng Luo Jingwei Zhu Yi Luo Shengqiang Ren Xia Hao Lili Wu Jingquan Zhang Dewei Zhao Wanhai Wang Weihua Tang Felix Lang Jarla Thiesbrummel Sahil Shah Martin Stolterfoht Kun Wei Jinbao Zhang Changlei Wang Huagui Lai Fan Fu Hao Huang Bingsuo Zou Jie Zhou Xinxing Yin College of Materials Science and Engineering & Institute of New Energy and Low-Carbon Technology Engineering Research Center of Alternative Energy Materials & Devices Ministry of Education Sichuan University Chengdu China Institute of Flexible Electronics (IFE Future Technologies) & Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM) Xiamen University Xiamen China School of Chemical Engineering Nanjing University of Science and Technology Nanjing China Institute of Physics and Astronomy University of Potsdam Karl-Liebknecht-Str. 24–25 Potsdam-Golm Germany Clarendon Laboratory University of Oxford Parks Road Oxford UK College of Materials Fujian Key Laboratory of Advanced Materials Xiamen Key Laboratory of Electronic Ceramic Materials and Devices Xiamen University Xiamen China School of Optoelectronic Science and Engineering & Collaborative Innovation Center of Suzhou Nano Science and Technology Key Lab of Advanced Optical Manufacturing Technologies of Jiangsu Province & Key Lab of Modern Optical Technologies of Education Ministry of China Soochow University Suzhou China Laboratory for Thin Films and Photovoltaics Empa - Swiss Federal Laboratories for Materials Science and Technology Duebendorf Switzerland State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures & School of Resources Environment and Materials Guangxi University Nanning China China-Australia Institute for Advanced Materials and Manufacturing (IAMM) Jiaxing University Jiaxing China

All-perovskite tandem solar cells (TSCs) promise high power conversion efficiency at a low cost1-4. Rapid efficiency improvement in small-area (1.75 eV) perovskite top subcells8, which currently suffer from large volt...

All-perovskite tandem solar cells (TSCs) promise high power conversion efficiency at a low cost1-4. Rapid efficiency improvement in small-area (<0.1 cm2) TSCs has been primarily driven by advances in low-bandgap (~1.25 eV) perovskite bottom subcells5-7. However, unsolved issues remain for wide-bandgap (WBG, >1.75 eV) perovskite top subcells8, which currently suffer from large voltage and fill factor (FF) losses, particularly for large-area (>1 cm2) TSCs. Here we develop a novel self-assembled monolayer (4-(7H-dibenzo[c,g]carbazol-7-yl)butyl)phosphonic acid (4PADCB) as a hole selective layer for WBG perovskite solar cells (PSCs), which facilitates subsequent growth of high-quality WBG perovskite over a large area with suppressed interfacial non-radiative recombination, enabling efficient hole extraction. Integrating 4PADCB in devices, we demonstrate a high open-circuit voltage (VOC) of 1.31 V in a 1.77-eV PSC, corresponding to a record lowVOC-deficit of 0.46 V (with respect to the bandgap). With these WBG perovskite subcells, we report 27.0% (26.4% certified stabilized) monolithic all-perovskite TSCs with an aperture area of 1.044 cm2. The certified tandem cell shows an outstanding combination of a highVOCof 2.12 V and a FF of 82.6%. Our demonstration of the large-area TSCs with certified record efficiency is a key step toward upscaling all-perovskite tandem photovoltaic technology.

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Deciphering Structure-Activity Relationship Towards CO2Electroreduction over SnO2by A Standard Research Paradigm

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Angewandte Chemie 2024年第12期136卷

作者： Zhongyuan Guo Yihong Yu Congcong Li Egon Campos dos Santos Tianyi Wang Huihui Li Prof. Jiang Xu Prof. Chuangwei Liu Prof. Hao Li College of Environmental and Resource Sciences Zhejiang University Hangzhou 310058 China Advanced Institute for Materials Research (WPI-AIMR) Tohoku University Sendai 980-8577 Japan The authors contribute equally to the work. Key Lab for Anisotropy and Texture of Materials School of Materials Science and Engineering Northeastern University Shenyang 110819 China Key Laboratory for Ultrafine Materials of Ministry of Education School of Chemical Engineering East China University of Science and Technology Shanghai 200237 China State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 China

Authentic surface structures under reaction conditions determine the activity and selectivity of electrocatalysts, therefore, the knowledge of the structure-activity relationship can facilitate the design of efficient catalyst structures for specific reactivity requirements. However, understanding the relationship between a more realistic active surface and its performance is challenging due to the complicated interface microenvironment in electrocatalysis. Herein, we proposed a standard research paradigm to effectively decipher the structure-activity relationship in electrocatalysis, which is exemplified in the CO 2 electroreduction over SnO 2 . The proposed practice has aided in discovering authentic/resting surface states (Sn layer) of SnO 2 accountable for the electrochemical CO 2 reduction reaction (CO 2 RR) performance under electrocatalytic conditions, which then is corroborated in the subsequent CO 2 RR experiments over SnO 2 with different morphologies (nanorods, nanoparticles, and nanosheets) in combination with in situ characterizations. This proposed methodology is further extended to the SnO electrocatalysts, providing helpful insights into catalytic structures. It is believed that our proposed standard research paradigm is also applicable to other electrocatalytic systems, in the meantime, decreases the discrepancy between theory and experiments, and accelerates the design of catalyst structures that achieve sustainable performance for energy conversion.

关键词： Standard research paradigm Surface states Surface reconstruction SnO2 CO2RR

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engineering a Local Free Water Enriched Microenvironment for Surpassing Platinum Hydrogen Evolution Activity

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Angewandte Chemie 2022年第35期134卷

作者： Qunlei Wen Junyuan Duan Wenbin Wang Dr. Danji Huang Dr. Youwen Liu Dr. Yongliang Shi Prof. JiaKun Fang Prof. Anmin Nie Prof. Huiqiao Li Prof. Tianyou Zhai State Key Laboratory of Materials Processing and Die & Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 P. R. China Contribution: Conceptualization (equal) Investigation (lead) Writing - original draft (lead) Contribution: Formal analysis (equal) Investigation (equal) Contribution: Investigation (supporting) Writing - original draft (supporting) State Key Lab of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 P. R. China Contribution: Formal analysis (supporting) Investigation (supporting) Contribution: Conceptualization (lead) Formal analysis (lead) Writing - review & editing (lead) Center for Spintronics and Quantum Systems State Key Laboratory for Mechanical Behavior of Materials School of Materials Science and Engineering Xi'an Jiaotong University Xi'an Shanxi 710049 P. R. China Contribution: Investigation (lead) Writing - review & editing (equal) Contribution: Conceptualization (supporting) Formal analysis (equal) Investigation (equal) Writing - review & editing (equal) Center for High Pressure Science State Key Laboratory of Metastable Materials Science and Technology Yanshan University Qinhuangdao Hebei 066004 P. R. China Contribution: Formal analysis (equal) Contribution: Writing - review & editing (equal) Contribution: Conceptualization (supporting) Project administration (lead) Supervision (equal) Writing - review & editing (equal)

Manipulating the catalyst–electrolyte interface to push reactants into the inner Helmholtz plane (IHP) is highly desirable for efficient electrocatalysts, however, it has rarely been implemented due to the elusive electrochemical IHP and inherent inert catalyst surface. Here, we propose the introduction of local force fields by the surface hydroxyl group to engineer the electrochemical microenvironment and enhance alkaline hydrogen evolution activity. Taking a hydroxyl group immobilized Ni/Ni 3 C heterostructure as a prototype, we reveal that the local hydrogen bond induced by the surface hydroxyl group drags 4-coordinated hydrogen-bonded H 2 O molecules across the IHP to become free H 2 O and thus continuously supply reactants forcatalytic sites catalytic sites. In addition, the hydroxyl group coupled with the Ni/Ni 3 C heterostructure further lowers the water dissociation energy by polarization effects. As a direct outcome, hydroxyl-rich catalysts surpass Pt/C activity at high current density (500 mA cm −2 @ ≈276 mV) in alkaline medium.

关键词： Electrochemical Double Layer High Current Densities Hydrogen Evolution Local Hydrogen Bond Surface Hydroxyl

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Tandem Catalysis for Selective Oxidation of Methane to Oxygenates Using Oxygen over PdCu/Zeolite

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Angewandte Chemie 2022年第24期134卷

作者： Bo Wu Tiejun Lin Min Huang Shenggang Li Ji Li Xing Yu Ruoou Yang Fanfei Sun Zheng Jiang Yuhan Sun Liangshu Zhong CAS Key Laboratory of Low-Carbon Conversion Science and Engineering Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201210 P. R. China University of Chinese Academy of Sciences Beijing 100049 P. R. China School of Physical Science and Technology ShanghaiTech University Shanghai 201210 P. R. China Shanghai Synchrotron Radiation Facility Zhangjiang National Lab Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 P. R. China State Key Laboratory of Materials Processing and Die & Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 P. R. China

Selective oxidation of methane to oxygenates with O 2 under mild conditions remains a great challenge. Here we report a ZSM-5 (Z-5) supported PdCu bimetallic catalyst (PdCu/Z-5) for methane conversion to oxygenates by reacting with O 2 in the presence of H 2 at low temperature (120 °C). Benefiting from the co-existence of PdO nanoparticles and Cu single atoms via tandem catalysis, the PdCu/Z-5 catalyst exhibited a high oxygenates yield of 1178 mmol g −1 Pd h −1 (mmol of oxygenates per gram Pd per hour) and at the same time high oxygenates selectivity of up to 95 %. Control experiments and mechanistic studies revealed that PdO nanoparticles promoted the in situ generation of H 2 O 2 from O 2 and H 2 , while Cu single atoms not only accelerated the activation of H 2 O 2 for the generation of abundant hydroxyl radicals (⋅OH) from H 2 O 2 decomposition, but also enabled the homolytic cleavage of CH 4 by ⋅OH to methyl radicals (⋅CH 3 ). Subsequently, the ⋅OH reacted quickly with the ⋅CH 3 to form CH 3 OH with high selectivity.

关键词： Methane Oxygenates Reaction Mechanisms Selective Oxidation Tandem Catalysis

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