Highly Dispersive Cerium Atoms on Carbon Nanowires as Oxygen Reduction Reaction Electrocatalysts for Zn-Air Batteries.

Highly efficient noble-metal-free electrocatalysts for oxygen reduction reaction (ORR) are essential to reduce the costs of fuel cells and metal-air batteries. Herein, a single-atom Ce-N-C catalyst, constructed of atomically dispersed Ce anchored on N-doped porous carbon nanowires, is proposed to boost the ORR. This catalyst has a high Ce content of 8.55 wt % and a high activity with ORR half-wave potentials of 0.88 V in alkaline media and 0.75 V in acidic electrolytes, which are comparable to widely studied Fe-N-C catalysts. A Zn-air battery based on this material shows excellent performance and durability. Density functional theory calculations reveal that atomically dispersed Ce with adsorbed hydroxyl species (OH) can significantly reduce the energy barrier of the rate-determining step resulting in an improved ORR activity.

[1]  Zifeng Yan,et al.  Boosting the bifunctional oxygen electrocatalytic performance of atomically dispersed Fe site via atomic Ni neighboring , 2020 .

[2]  Qiang Xu,et al.  Single-Atom Iron Catalysts on Overhang-Eave Carbon Cages for High-Performance Oxygen Reduction Reaction. , 2020, Angewandte Chemie.

[3]  Dong Liu,et al.  Stabilizing Single-Atom Iron Electrocatalysts for Oxygen Reduction via Ceria Confining and Trapping , 2020 .

[4]  Yuehe Lin,et al.  Single-Atom Nanozyme Based on Nanoengineered Fe-N-C Catalyst with Superior Peroxidase-Like Activity for Ultrasensitive Bioassays. , 2019, Small.

[5]  Jin Zhao,et al.  Climbing the Apex of the ORR Volcano Plot via Binuclear Site Construction: Electronic and Geometric Engineering. , 2019, Journal of the American Chemical Society.

[6]  R. Behm,et al.  Chemical and Electronic Changes of the CeO2 Support during CO Oxidation on Au/CeO2 Catalysts: Time-Resolved Operando XAS at the Ce LIII Edge , 2019, Catalysts.

[7]  Changpeng Liu,et al.  Single-Atom Cr-N4 Sites Designed for Durable Oxygen Reduction Catalysis in Acid Media. , 2019, Angewandte Chemie.

[8]  Xiaoqing Pan,et al.  Secondary-Atom-Assisted Synthesis of Single Iron Atoms Anchored on N-Doped Carbon Nanowires for Oxygen Reduction Reaction , 2019, ACS Catalysis.

[9]  Jing Li,et al.  Atomic Fe‐Doped MOF‐Derived Carbon Polyhedrons with High Active‐Center Density and Ultra‐High Performance toward PEM Fuel Cells , 2019, Advanced Energy Materials.

[10]  Hong‐Jie Peng,et al.  From Supramolecular Species to Self-Templated Porous Carbon and Metal-Doped Carbon for Oxygen Reduction Reaction Catalysts. , 2019, Angewandte Chemie.

[11]  Song Gao,et al.  Puffing Up Energetic Metal-Organic Frameworks to Large Carbon Networks with Hierarchical Porosity and Atomically Dispersed Metal Sites. , 2019, Angewandte Chemie.

[12]  Chang Liu,et al.  Carbon nanotube encapsulated in nitrogen and phosphorus co-doped carbon as a bifunctional electrocatalyst for oxygen reduction and evolution reactions , 2018, Carbon.

[13]  D. Cullen,et al.  Atomically dispersed manganese catalysts for oxygen reduction in proton-exchange membrane fuel cells , 2018, Nature Catalysis.

[14]  L. Dai,et al.  Efficient Oxygen Reduction Reaction (ORR) Catalysts Based on Single Iron Atoms Dispersed on a Hierarchically Structured Porous Carbon Framework. , 2018, Angewandte Chemie.

[15]  Qianwang Chen,et al.  O‐, N‐Atoms‐Coordinated Mn Cofactors within a Graphene Framework as Bioinspired Oxygen Reduction Reaction Electrocatalysts , 2018, Advanced materials.

[16]  Hao Ming Chen,et al.  A Universal Method to Engineer Metal Oxide-Metal-Carbon Interface for Highly Efficient Oxygen Reduction. , 2018, ACS nano.

[17]  D. Su,et al.  Microporous Framework Induced Synthesis of Single-Atom Dispersed Fe-N-C Acidic ORR Catalyst and Its in Situ Reduced Fe-N4 Active Site Identification Revealed by X-ray Absorption Spectroscopy , 2018 .

[18]  M. Roeffaers,et al.  Unravelling the Redox-catalytic Behavior of Ce4+ Metal-Organic Frameworks by X-ray Absorption Spectroscopy. , 2018, Chemphyschem : a European journal of chemical physics and physical chemistry.

[19]  J. Baek,et al.  Defect-Free Encapsulation of Fe0 in 2D Fused Organic Networks as a Durable Oxygen Reduction Electrocatalyst. , 2018, Journal of the American Chemical Society.

[20]  Chang Liu,et al.  N-doped carbon nanotubes containing a high concentration of single iron atoms for efficient oxygen reduction , 2018 .

[21]  S. Shanmugam,et al.  A synergistic effect of Co and CeO2 in nitrogen-doped carbon nanostructure for the enhanced oxygen electrode activity and stability , 2017, Applied Catalysis B: Environmental.

[22]  Chengzhou Zhu,et al.  Single-Atom Electrocatalysts. , 2017, Angewandte Chemie.

[23]  Chang Liu,et al.  Heteroatom-Doped Carbon Nanotube and Graphene-Based Electrocatalysts for Oxygen Reduction Reaction. , 2017, Small.

[24]  Yuyan Shao,et al.  Single Atomic Iron Catalysts for Oxygen Reduction in Acidic Media: Particle Size Control and Thermal Activation. , 2017, Journal of the American Chemical Society.

[25]  R. Boukherroub,et al.  Efficient and Durable Oxygen Reduction Electrocatalyst Based on CoMn Alloy Oxide Nanoparticles Supported Over N-Doped Porous Graphene , 2017 .

[26]  L. Gu,et al.  Zn Single Atom Catalyst for Highly Efficient Oxygen Reduction Reaction , 2017 .

[27]  Yadong Li,et al.  Isolated Single Iron Atoms Anchored on N-Doped Porous Carbon as an Efficient Electrocatalyst for the Oxygen Reduction Reaction. , 2017, Angewandte Chemie.

[28]  S. Qiao,et al.  Recent Advances in Atomic Metal Doping of Carbon-based Nanomaterials for Energy Conversion. , 2017, Small.

[29]  S. Qiao,et al.  Surface and Interface Engineering of Noble-Metal-Free Electrocatalysts for Efficient Energy Conversion Processes. , 2017, Accounts of chemical research.

[30]  S. Mukerjee,et al.  Asymmetric Volcano Trend in Oxygen Reduction Activity of Pt and Non-Pt Catalysts: In Situ Identification of the Site-Blocking Effect. , 2017, Journal of the American Chemical Society.

[31]  Fuqiang Huang,et al.  Efficient catalyst of defective CeO2−x and few-layer carbon hybrid for oxygen reduction reaction , 2016 .

[32]  Fuzhi Li,et al.  Co3O4-CeO2/C as a Highly Active Electrocatalyst for Oxygen Reduction Reaction in Al-Air Batteries. , 2016, ACS applied materials & interfaces.

[33]  The Enhancement of Surface Reactivity on CeO2 (111) Mediated by Subsurface Oxygen Vacancies , 2016 .

[34]  Chang Liu,et al.  Hierarchically porous Fe-N-doped carbon nanotubes as efficient electrocatalyst for oxygen reduction , 2016 .

[35]  Yadong Li,et al.  Single Cobalt Atoms with Precise N-Coordination as Superior Oxygen Reduction Reaction Catalysts. , 2016, Angewandte Chemie.

[36]  Litao Sun,et al.  Elemental superdoping of graphene and carbon nanotubes , 2016, Nature Communications.

[37]  Jean-Pol Dodelet,et al.  Recent Advances in Electrocatalysts for Oxygen Reduction Reaction. , 2016, Chemical reviews.

[38]  Cuiling Zhang,et al.  Controlled growth cerium oxide nanoparticles on reduced graphene oxide for oxygen catalytic reduction , 2016 .

[39]  Edward F. Holby,et al.  Experimental Observation of Redox-Induced Fe-N Switching Behavior as a Determinant Role for Oxygen Reduction Activity. , 2015, ACS nano.

[40]  S. Mukerjee,et al.  Highly active oxygen reduction non-platinum group metal electrocatalyst without direct metal–nitrogen coordination , 2015, Nature Communications.

[41]  E. Holby,et al.  Activity of N-coordinated multi-metal-atom active site structures for Pt-free oxygen reduction reaction catalysis: Role of *OH ligands , 2015, Scientific Reports.

[42]  Tao Zhang,et al.  Single-atom catalysts: a new frontier in heterogeneous catalysis. , 2013, Accounts of chemical research.