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Chem Catalysis
This journal offers authors two options (open access or subscription) to publish research

Sep 15, 2022

Volume 2Issue 9p2109-2390
On the cover: Confining Cu atoms into the lattice of ultrathin Ru nanosheets achieves highly efficient CH4 conversion to liquid C1 oxygenates over the catalyst under room temperature (25°C). Multiple spectroscopic analyses and first-principle calculations reveal that Ru-edge-confined atomically dispersed Cu sites render high intrinsic activity. The work by Deng and colleagues (page 2253) presents a strategy for designing efficient catalysts by constructing confined active centers in metallic nanosheets for the activation of C–H bonds in light alkanes....
On the cover: Confining Cu atoms into the lattice of ultrathin Ru nanosheets achieves highly efficient CH4 conversion to liquid C1 oxygenates over the catalyst under room temperature (25°C). Multiple spectroscopic analyses and first-principle calculations reveal that Ru-edge-confined atomically dispersed Cu sites render high intrinsic activity. The work by Deng and colleagues (page 2253) presents a strategy for designing efficient catalysts by constructing confined active centers in metallic nanosheets for the activation of C–H bonds in light alkanes.

In This Issue

  • In this issue

    In This Issue highlights the most exciting articles of the current issue with short editorial pieces written by the corresponding handling editors.

Activity

  • Accurate synthesis and industrial production of single-atom catalysts

    • Jiarui Yang,
    • Jiajing Pei,
    • Juncai Dong,
    • Dingsheng Wang
    In this Activity article, the groups of Dingsheng Wang (professor in the Department of Chemistry at Tsinghua University) and Juncai Dong (distinguished research fellow of the Beijing Synchrotron Radiation Facility at the Institute of High Energy Physics) exchange views on accurate synthesis and large-scale application for single-atom catalysts.
  • Combining experiment and theory for precise structure identification of single-atom catalysts

    • Jiangwen Liao,
    • Jiarui Yang,
    • Dingsheng Wang,
    • Juncai Dong
    In this Activity article, the groups of Juncai Dong (distinguished research fellow of the Beijing Synchrotron Radiation Facility at the Institute of High Energy Physics) and Dingsheng Wang (professor in the Department of Chemistry at Tsinghua University) discuss the strengths and limitations of different advanced techniques used for fine-structure identification of single-atom catalysts and the opportunities for industry and academia to develop new efficient techniques and methodologies.

Previews

Perspectives

  • Boosting electrocatalytic water splitting by magnetic fields

    • Xiaoning Li,
    • Zhenxiang Cheng
    Magnetic fields will perform more than ever thought on the efficiency improvements of various energy-conversion reactions. According to the physical basis, the effects of the magnetic field on water electrolysis are classified to the magnetohydrodynamic effect in the electrolyte, the spin-selective effect in the interface, and the spin alignment and magnetothermal effects in electrocatalysts. With a comprehensive understanding of the underlying mechanisms, it is hoped we could find effective solutions to the issues in the clean-energy fields.
  • Carbon-based metal-free electrocatalysts: Recent progress and forward looking

    • Chuangang Hu,
    • Yuyang Gao,
    • Linjie Zhao,
    • Liming Dai
    The advances in research and development of carbon-based electrocatalysts have opened up new areas for metal-free electrocatalysis. This article provides an overview on the recent progress and future perspective of carbon-based metal-free electrocatalysts for various energy/chemical-related reactions. Current challenges and future opportunities in this rapidly developing field are also discussed.

Reviews

  • Covalent organic frameworks: Fundamentals, mechanisms, modification, and applications in photocatalysis

    • Zizhan Liang,
    • Rongchen Shen,
    • Yun Hau Ng,
    • Yang Fu,
    • Tianyi Ma,
    • Peng Zhang,
    • Youji Li,
    • Xin Li
    This review highlights four important aspects for rationally and precisely designing highly efficient and selective COF-based photocatalysts, in the sequence of considerate design principles based on the understanding of photocatalytic fundamentals, deep insights into the photocatalytic mechanisms, diversified synthesis and engineering-modification strategies, and significant and urgent points in different emerging applications.
  • Interfacial electric field effect on electrochemical carbon dioxide reduction reaction

    • Jinli Yu,
    • Jinwen Yin,
    • Ruchun Li,
    • Yangbo Ma,
    • Zhanxi Fan
    The electrochemical carbon dioxide (CO2)reduction reaction is of great significance in cutting CO2 emissions and achieving carbon neutrality. Recent studies have observed that the interfacial electric field controlled by cations, morphology, and additives has profound effects on the thermodynamics and kinetics of electrochemical CO2 reduction processes. Herein, we provide a comprehensive review of the interfacial electric field effects on electrochemical CO2 reduction reaction.

Articles

    Featured Article
  • Boosting room-temperature conversion of methane via confining Cu atoms in ultrathin Ru nanosheets

    • Jinchang Fan,
    • Suxia Liang,
    • Kaixin Zhu,
    • Jun Mao,
    • Xiaoju Cui,
    • Chao Ma,
    • Liang Yu,
    • Dehui Deng
    Room-temperature methane conversion to liquid C1 oxygenates is achieved over ultrathin Ru nanosheets with confined Cu atoms. Bi-coordinated bridge-site oxygen species generated on the Ru edge-confined Cu sites are revealed as the active centers to convert methane via a free radical mechanism.
  • Producing ultrastable Ni-ZrO2 nanoshell catalysts for dry reforming of methane by flame synthesis and Ni exsolution

    • Shuo Liu,
    • Chaochao Dun,
    • Mihir Shah,
    • Junjie Chen,
    • Satyarit Rao,
    • Jilun Wei,
    • Eleni A. Kyriakidou,
    • Jeffrey J. Urban,
    • Mark T. Swihart
    A highly stable Ni-ZrO2 nanoshell catalyst is produced by a continuous flame aerosol process and Ni exsolution. Its notable characteristics include abundant oxygen vacancies and strong metal-support interactions, which lead to both coking and sintering resistance, along with high activity, for dry reforming of methane.
  • Single Nb atom modified anatase TiO2(110) for efficient electrocatalytic nitrogen reduction reaction

    • Yunnan Gao,
    • Yang Yang,
    • Leiduan Hao,
    • Song Hong,
    • Xinyi Tan,
    • Tai-Sing Wu,
    • Yun-Liang Soo,
    • Alex W. Robertson,
    • Qi Yang,
    • Zhenyu Sun
    Ammonia is extensively used in industry, agriculture, and energy storage. Currently, the industrial synthesis of ammonia predominantly still relies on the energy- and capital-intensive Haber-Bosch (HB) process. Electrochemical N2 reduction reaction (NRR) provides a renewable and distributed route for ammonia production. To boost the NRR, the development of electrocatalysts is key. Herein, we design and synthesize Nb single-atom-decorated anatase TiO2(110) for enhanced NRR, affording an NH3 production rate of ∼21.3 μg h−1 mgcat−1.
  • Toward gasoline vehicles with zero harmful emissions by storing NO at Pd nanoparticle–CeO2 interface during the cold-start period

    • Jaeha Lee,
    • Yongwoo Kim,
    • Sungha Hwang,
    • Gwang Seok Hong,
    • Eunwon Lee,
    • Hyokyoung Lee,
    • Changho Jeong,
    • Chang Hwan Kim,
    • Jong Suk Yoo,
    • Do Heui Kim
    A method for maximizing NO abatement by combining the catalytic function of Pd/CeO2 and switching the air-fuel ratio by engine control is suggested. Pd nanoparticles were loaded onto CeO2, forming oxygen vacancies that temporarily stored NO gas to mitigate NO emissions during the cold-start period of gasoline vehicles, and it is maximized by engine control. Combined experimental and theoretical studies further reveal NO storage mechanism and the role of Pd nanoparticles and CeO2.
  • Biomass-based production of food preservatives

    • Lin Yuan,
    • Yancheng Hu,
    • Xin Guo,
    • Guangyi Li,
    • Aiqin Wang,
    • Yu Cong,
    • Feng Wang,
    • Tao Zhang,
    • Ning Li
    Sorbate and benzoate are the two most important preservatives in the food and beverage industry. Currently, they are manufactured from fossil-derived ketene and toluene, respectively. To reduce dependence on non-renewable energy, Yuan et al. exploit alternative routes to access preservatives using biomass-based malonate, crotonaldehyde, and acrolein as the starting materials. Life-cycle assessment indicates that our biobased routes release less greenhouse gases than their traditional synthesis.
  • Unraveling Ni-Fe 2D nanostructure with enhanced oxygen evolution via in situ and operando spectroscopies

    • Young-Jin Ko,
    • Man Ho Han,
    • Haesol Kim,
    • Jun-Yong Kim,
    • Woong Hee Lee,
    • Jaewook Kim,
    • Joon Young Kwak,
    • Chang-Hee Kim,
    • Tae-Eon Park,
    • Seung-Ho Yu,
    • Wook-Seong Lee,
    • Chang Hyuck Choi,
    • Peter Strasser,
    • Hyung-Suk Oh
    Open Access
    Oh and co-workers have prepared an ultrathin Ni-Fe layered double hydroxide via a facile route and suggest a synthetic mechanism to form thin layers. On the basis of detailed in situ and operando analyses, they reveal that the phase transformation occurs as soon as contact is established with electrolyte without applied potential. By proposing the oxygen evolution reaction (OER) mechanism and measuring oxygen evolution performance, the authors clearly present the future path of progression for the water electrolysis catalyst.
  • Illustrating the overall reaction network of the synthesis-gas-to-hydrocarbons process over iron-zeolite bifunctional catalysis

    • Xuan Gong,
    • Adrian Ramirez,
    • Edy Abou-Hamad,
    • Tuiana B. Shoinkhorova,
    • Mustafa Çağlayan,
    • Yiru Ye,
    • Wei Wang,
    • Nimer Wehbe,
    • Rushana Khairova,
    • Abhishek Dutta Chowdhury,
    • Jorge Gascon
    Identifying “descriptor”-style carbon-based reaction intermediates is significant in upgrading the current state of metal-zeolite bifunctional “cascade” catalysis. In this work, four different product selectivities (short olefins, light paraffins, long-chain hydrocarbons, and aromatics) were observed during the syngas-to-hydrocarbon process (Fischer-Tropsch type) over potassium superoxide-doped iron oxide/zeolite-based bifunctional catalysts. Here, we demonstrate that the zeolite topology and “co-catalytic” hybrid supramolecular reactive centers (i.e., organic hydrocarbons pool species trapped by the inorganic zeolite) regulate the reaction mechanism and the final product selectivity.
  • Atomically dispersed 3d metal bimetallic dual-atom catalysts and classification of the structural descriptors

    • Ching Kit Tommy Wun,
    • Ho Kit Mok,
    • Tianxiang Chen,
    • Tai-Sing Wu,
    • Keita Taniya,
    • Keizo Nakagawa,
    • Sarah Day,
    • Chiu C. Tang,
    • Ziru Huang,
    • Haibin Su,
    • Wing-Yiu Yu,
    • Terence Kin Wah Lee,
    • Tsz Woon Benedict Lo
    The manipulation and control of materials and phenomena at atomic and molecular dimensions are achieved by utilizing the fundamental concepts of coordination and solid-state chemistries. The findings presented in this work reveal the precise engineering of supported dual-atom catalysts (such as combinations of 3d/4d metals) over support materials not only for biochemical applications but also for more extensive applications. This shall genuinely bring heterogeneous catalysis toward the molecular frontier that addresses the critical challenges in the field.
  • The effect of flue gas contaminants on electrochemical reduction of CO2 to methyl formate in a dual methanol/water electrolysis system

    • Manu Gautam,
    • Dillon T. Hofsommer,
    • Sandesh S. Uttarwar,
    • Nolan Theaker,
    • William F. Paxton,
    • Craig A. Grapperhaus,
    • Joshua M. Spurgeon
    The feasibility of electrochemical reduction of waste carbon dioxide from industrial flue gas was investigated in an uncommon methanol/water dual electrolyte approach targeting a methyl formate product. The work demonstrates a pathway to produce a chemical not formed in aqueous CO2 reduction that is largely compatible with direct operation from flue gas.
  • Featured Article
  • Copper-catalyzed hydroamination of polyfluoroalkyl substituted alkenes via asymmetric radical cross-coupling access to α-chiral tertiary alkylamines

    • Yu-Jie Liang,
    • Meng-Jiao Sun,
    • Ge Zhang,
    • Jian-Jun Yin,
    • Wei Guan,
    • Tao Xiong,
    • Qian Zhang
    A Cu-catalyzed radical cross-coupling of in-situ-generated Cu(I)-bounded dialkyl amine radical species with a carbon-based radical species to create a chiral C–N bond has been disclosed for the first time to our knowledge. By virtue of this approach, asymmetric radical hydroamination of β-aryl substituted polyfluoroalkyl alkenes with hydroxylamine derivatives has been successfully implemented to access an array of important β-polyfluoroalkyl substituted α-chiral tertiary alkylamines in an excellent regio- and enantioselective manner.
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