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Article
Chemistry, Multidisciplinary
Feifei Zhang et al.
Summary: A new type of W SAC with unique local structure was designed and prepared, showing excellent performance in electrochemical ORR, particularly in terms of H2O2 selectivity and operational durability. The findings open up new opportunities for developing high-performance W-based catalysts for electrochemical H2O2 production.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Haisheng Gong et al.
Summary: By simultaneously regulating the coordination number of atomically dispersed cobalt sites and nearby oxygen functional groups through a one-step microwave thermal shock, a highly selective and active Co-N-C electrocatalyst for H2O2 electrosynthesis has been obtained. This catalyst exhibits high H2O2 selectivity, outstanding mass activity, and large kinetic current density, showing great potential for the development of new electrocatalysts with unprecedented reactivity.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Zheng Zhou et al.
Summary: Electrocatalytic hydrogen peroxide synthesis via two-electron oxygen reduction reaction pathway is becoming increasingly important due to its green production process. Introducing cationic vacancies on nickel phosphide as a proof-of-concept to regulate the catalyst's properties has led to efficient H2O2 electrosynthesis. The created Ni cationic vacancies enriched Ni2-xP-V-Ni electrocatalyst exhibits remarkable 2e ORR performance and long-term durability, with optimized geometric and electronic structures. Cation vacancy engineering is believed to be an effective strategy for creating active heterogeneous catalysts with atomic precision.
ADVANCED MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Erhuan Zhang et al.
Summary: Rarely reported is the in-depth understanding of local atomic environment-property relationships of p-block metal single-atom catalysts towards the 2e(-) oxygen reduction reaction (ORR). In this study, a heteroatom-modified In-based metal-organic framework-assisted approach is developed to synthesize an optimal catalyst, In SAs/NSBC, with accurately anchored single In atoms supported by hollow carbon rods. The catalyst exhibits a high H2O2 selectivity and unprecedented production rates in different electrolytes, providing practical guidance for H2O2 electrosynthesis and enabling the design of high-performance single-atom materials.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Xueying Cao et al.
Summary: By utilizing the electrospun-pyrolysis cooperative strategy to modulate the porous structure of the carbon support and adjust the bridging structure of atomically dispersed metal species, the unique chemical structure of binuclear nickel bridging with nitrogen and carbon atoms has been identified to enhance CO2 reduction substantially.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Yaling Jia et al.
Summary: Accurately regulating the selectivity of the oxygen reduction reaction (ORR) by tailoring the coordination environment of atomically dispersed Zn sites can achieve high selectivity, with ZnO3C catalyst processing a 2 e(-) ORR pathway for H2O2 generation in 0.1 M KOH. This is attributed to the decreased electron density around Zn in ZnO3C which changes the intermediate adsorption and contributes to the high selectivity towards 2 e(-) ORR.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Xiaogang Li et al.
Summary: The study shows that confining isolated metal sites on carbon supports can increase the selectivity of aminoanthraquinone as a catalyst in catalyzing the oxygen reduction reaction to produce H2O2. By reducing the thermodynamic barrier for OOH* desorption, the selectivity for H2O2 is improved.
ADVANCED MATERIALS
(2022)
Review
Chemistry, Multidisciplinary
Shenlong Zhao et al.
Summary: Studying the structure-activity correlations of electrocatalysts is crucial for improving the conversion of electrical to chemical energy. Recent evidence obtained through operando characterization techniques shows that the structural evolution of catalysts, caused by their interaction with electric fields, electrolytes, and reactants/intermediates, leads to the formation of real active sites. It is therefore important to summarize the research advances in structural evolution and envision future developments. In this Minireview, the fundamental concepts associated with structural evolution, the triggers of this evolution, and advanced operando characterizations are discussed. The reversibility of structural evolution in heterogeneous electrocatalysis, with a focus on the oxygen evolution and CO2 reduction reactions, is also highlighted. Finally, the key challenges and opportunities in this exciting field are presented.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Kuang-Hsu Wu et al.
Summary: Modulating the steric-electronic configuration of metal-organic centers is key for tuning the activity and selectivity of heterogeneous reactions. In this study, three different asymmetric metal-organic complexes with unique steric-electronic structures are immobilized on nanocarbon for an electron-transfer-controlled oxygen reduction reaction. The results show that acidic diamine ligands facilitate a four-electron transfer, while basic ligands drive a highly selective two-electron route, regulated by the ligand's proton transfer ability.
Article
Chemistry, Multidisciplinary
Fan Xiao et al.
Summary: A new strategy of generating hydroxyl radicals from electrocatalytic reduction of oxygen has been reported, showing fast and complete removal of ciprofloxacin with high degradation rate and stability. This approach involves tuning the electronic environment to regulate electrocatalytic activity, achieving results comparable to state-of-the-art advanced oxidation processes.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Lei Zhang et al.
Summary: Cu(I)-based catalysts are essential for the electrocatalytic CO2 reduction, and in this study, two stable copper(I)-based catalysts with inherent cuprophilic interactions were synthesized for highly selective CO2-to-CH4 conversion. The substitution of sulfate radicals with hydroxyl radicals led to a dynamic crystal structure transition, enhancing the cuprophilic interactions inside the catalyst structure. The enhanced cuprophilic interactions in NNU-33(H) showed outstanding CH4 selectivity, representing the best crystalline catalyst for electrocatalytic CO2-to-CH4 conversion.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Peike Cao et al.
Summary: A highly hydrophobic gas-liquid-solid three-phase architecture has been proposed to improve the electrochemical synthesis of H2O2, achieving high efficiency and high concentration of H2O2 production.
Article
Chemistry, Multidisciplinary
Shanyong Chen et al.
Summary: A chemical titration strategy was proposed to decipher the mechanism of oxygen-doped carbon nanosheet catalyst for 2 e(-) ORR, revealing that C=O species are the main active sites for electrocatalytic activity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Cheng Tang et al.
Summary: This study demonstrates that the molecular-level local structure, including first and second coordination spheres, plays a critical role in determining the selectivity of catalytic reactions. By modifying the first and second coordination spheres of Co-SACs, it is possible to tailor the oxygen reduction reaction selectivity. The unique selectivity change originates from the structure-dependent shift of active sites, leading to improved activity and selectivity for acidic H2O2 electrosynthesis.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Fan Xia et al.
Summary: The Chevrel phase chalcogenide Ni2Mo6S8 is a novel active motif for reducing oxygen to H2O2, exhibiting exceptional activity with high selectivity, fast turnover frequencies, and stable crystal structure for continuous H2O2 production.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Hui Li et al.
Summary: Catalysts based on Cu nanocrystals with ultrathin Al2O3 overcoating show significantly improved selectivity and stability in electrochemical CO2-to-C2+ conversion, with a C2H4 faradaic efficiency as high as 60.4% at a current density of 300 mA cm(-2). The Al2O3 overcoating effectively suppresses the dynamic mobility and aggregation of Cu nanocrystals, leading to negligible activity loss during stability tests.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Yongguang Zhang et al.
Summary: In this study, a novel single atom catalyst and unique carbon support were synthesized to improve the performance of lithium-sulfur batteries, mitigate the shuttle effect of polysulfides, and enhance the kinetics of redox reactions, resulting in outstanding battery performance.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Yahui Wu et al.
Summary: Guided by first-principles calculations, it was discovered that Cd single-atom catalysts have excellent performance in activating CO2, and the introduction of axial coordination structure can further decrease the free energy barrier of CO2 reduction while suppressing the hydrogen evolution reaction. The designed and synthesized novel Cd SAC showed outstanding performance in CO2 electroreduction to CO, achieving a high faradaic efficiency and turnover frequency. This work serves as a successful example of designing highly efficient catalysts guided by theoretical calculations.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Multidisciplinary Sciences
Yang Xia et al.
Summary: Oxygen reduction reaction provides an environmentally-benign route for hydrogen peroxide production but lacks efficient catalysts to achieve high selectivity and activity simultaneously. Here, the authors report a boron-doped carbon catalyst which shows great promise with outstanding performance.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
Qinglan Zhao et al.
Summary: The study demonstrates the efficient production of H2O2 using cobalt single-atom catalysts in simulated seawater, showing long-term stability and high chloride-endurability. It reveals that the Co-N-5 structure is the main active site for H2O2 formation, offering a promising pathway for large-scale electrocatalytic oxygen reduction in simulated seawater towards energy sustainability.
ENERGY & ENVIRONMENTAL SCIENCE
(2021)
Article
Chemistry, Multidisciplinary
Zhiqiang Chen et al.
Summary: Through a fast-pyrolyzing and controllable-activation strategy, an O-rich carbonaceous support and atomically dispersed FeN4 site with axial O coordination were constructed, achieving a wide potential range and high FECO. DFT calculations revealed that the superior performance originated from the axial O-coordination induced electronic localization enhancement, facilitating CO desorption and increasing the energy barrier for competitive hydrogen evolution reaction.
ENERGY & ENVIRONMENTAL SCIENCE
(2021)
Article
Chemistry, Multidisciplinary
Xue Wang et al.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2020)
Article
Chemistry, Physical
Euiyeon Jung et al.
Article
Chemistry, Multidisciplinary
Yulin Wang et al.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2020)
Article
Multidisciplinary Sciences
Gao-Feng Han et al.
NATURE COMMUNICATIONS
(2020)
Article
Chemistry, Physical
Laiquan Li et al.
ADVANCED ENERGY MATERIALS
(2020)
Article
Multidisciplinary Sciences
Qingran Zhang et al.
NATURE COMMUNICATIONS
(2020)
Review
Materials Science, Multidisciplinary
Jiajian Gao et al.
ACS MATERIALS LETTERS
(2020)
Article
Chemistry, Multidisciplinary
Bo-Quan Li et al.
ADVANCED MATERIALS
(2019)
Article
Chemistry, Multidisciplinary
Huinian Zhang et al.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2019)
Article
Chemistry, Multidisciplinary
Yanyan Sun et al.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2019)
Article
Chemistry, Multidisciplinary
Bo‐Quan Li et al.
ADVANCED MATERIALS
(2019)
Article
Multidisciplinary Sciences
Chuan Xia et al.
Article
Multidisciplinary Sciences
Kun Jiang et al.
NATURE COMMUNICATIONS
(2019)
Article
Chemistry, Physical
Zhiyi Lu et al.
