Angew Chem Int Ed Engl
September 2025
The sustainable and widespread developments of fuel cells require material innovation toward the sluggish oxygen reduction reaction (ORR). Although iron and nitrogen co-doped carbon material (Fe-N-C) is a promising alternative to scarce and expensive platinum-based electrocatalysts, the linear scaling relationships among the intermediates' adsorption energy limit maximum performance. Herein, we propose a coordination-adaptive catalyst design to bypass the intrinsic scaling relations through incorporating quasi-covalent Fe─F bond.
View Article and Find Full Text PDFThe inherent scaling relationships between adsorption energies of oxygen-containing intermediates impose an intrinsic limitation on the maximum oxygen reduction reaction (ORR) activity, which represents one of the bottlenecks for the practical application of anion exchange membrane fuel cells (AEMFCs). To address this challenge, we align the 3dz orbital energy levels of Fe and Co to selectively customize the dissociative ORR pathway without the formation of OOH* intermediates, circumventing the conventional OH*-OOH* scaling relations. This rational design is achieved by atomic phosphorus(P) substitution, which not only optimizes orbital matching towards O-O cis-bridge adsorption, but also stabilizes the spontaneously adsorbed OH ligand as an electronic modifier.
View Article and Find Full Text PDFHeteronuclear dual-atoms catalysts (DACs) represent an emerging frontier in heterogeneous catalysis due to maximum atom utilization and synergistic catalysis, yet their precise synthesis remains challenging. Herein, we propose a universal "metal ion targeting coordination" (MITC) strategy to construct a series of heteronuclear DACs. This approach utilizes the bipyridyl (bpy) ligands to coordinate a primary metal (M), forming an artificial monooxygenase (bpy)M(μ-OH) structure, where electron-enriched oxygen atoms serve as anchoring sites for a secondary metal (M).
View Article and Find Full Text PDFSunlight-driven production of high-value chemicals from renewable resources represents a pivotal driver toward achieving sustainable energy supply. However, fundamental barriers include inadequate use of light energy and insufficient understanding of reactive oxygen species (ROS) regulating mechanisms in photocatalytic processes. To address this, a novel symbiotic strategy for the design of Cu/TiO single-atom catalysts (SACs) supported by density functional theory (DFT) calculations was proposed.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
March 2025
Fe-N-C catalysts, with a planar D symmetric FeN structure, show promising as noble metal-free oxygen reduction reaction catalysts. Nonetheless, the highly symmetric structure restricts the effective manipulation of its geometric and electronic structures, impeding further enhancements in oxygen reduction reaction performance. Here, a high proportion of asymmetric edge-carbon was successfully introduced into Fe-N-C catalysts through morphology engineering, enabling the precise modulation of the FeN active site.
View Article and Find Full Text PDFJ Synchrotron Radiat
July 2024
The BL17B beamline at the Shanghai Synchrotron Radiation Facility was first designed as a versatile high-throughput protein crystallography beamline and one of five beamlines affiliated to the National Facility for Protein Science in Shanghai. It was officially opened to users in July 2015. As a bending magnet beamline, BL17B has the advantages of high photon flux, brightness, energy resolution and continuous adjustable energy between 5 and 23 keV.
View Article and Find Full Text PDFJ Appl Crystallogr
June 2024
A general synthetic protocol is developed to afford a series of [MW12O44] (M = Ni2+, Co2+ and Fe3+) clusters with diverse central heteroatoms, by employing [W12O44]16- as the structure-directing precursor. The structures of the [MW12O44] clusters are definitively confirmed by single crystal X-ray diffraction (XRD). The central heteroatoms are monodispersed and capture the "empty" cavity of [W12O44]16- with an 8 coordination number state, as demonstrated by the combination of single crystal structure extended X-ray absorption fine structure (EXAFS) fitting analysis and wavelet transform EXAFS (WTEXAFS).
View Article and Find Full Text PDFNat Commun
September 2017
This corrects the article DOI: 10.1038/ncomms15938.
View Article and Find Full Text PDFFor the large-scale sustainable implementation of polymer electrolyte membrane fuel cells in vehicles, high-performance electrocatalysts with low platinum consumption are desirable for use as cathode material during the oxygen reduction reaction in fuel cells. Here we report a carbon black-supported cost-effective, efficient and durable platinum single-atom electrocatalyst with carbon monoxide/methanol tolerance for the cathodic oxygen reduction reaction. The acidic single-cell with such a catalyst as cathode delivers high performance, with power density up to 680 mW cm at 80 °C with a low platinum loading of 0.
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