In view of the outstanding catalytic efficiency, single-atom catalysts (SACs) have shown great promise for the construction of sensitive chemiluminescent (CL) platforms. However, the low loading amount of active sites dramatically obstructs the improved catalytic activity of these metal SACs. Benefiting from the exceedingly unique catalytic properties of the metal-metal bonds, atomic clusters may give rise to enhancing the catalytic properties of SACs based on the synergistic effects of dual atomic-scale sites. Inspired by this, atomic CoN clusters-assisted Co SACs (CoN@Co SACs) were synthesized through a facile doping method. Through X-ray absorption spectroscopy, the active metal sites in the synergetic dual-site atomic catalysts of CoN@Co SACs were confirmed to be Co-O and Co-N moieties. CoN@Co SACs served as a superior co-reactant to remarkably enhance the luminol CL signal by 2155.0 times, which was prominently superior to the boosting effect of the pure Co SACs (98.4 times). The synergetic dual-site atomic catalysts contributed to accelerating the decomposition of HO into singlet oxygen as well as superoxide radical anions to display superb catalytic performances. For a concept employment, CoN@Co SACs were attempted to utilize as CL probes for establishing a sensitive immunochromatographic assay to quantitate pesticide residues, in which imidacloprid was adopted as the model analyte. The quantitative range of imidacloprid was 0.05-10 ng mL with a detection limit of 1.7 pg mL (3σ). Furthermore, the satisfactory recovery values in mock herbal medicine samples demonstrated the effectiveness of the proposed CoN@Co SAC-based CL platform. In the proof-of-concept work, synergetic dual-site atomic catalysts show great perspectives on trace analysis and luminescent biosensing.
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http://dx.doi.org/10.1021/acs.analchem.2c02914 | DOI Listing |
Proc Natl Acad Sci U S A
February 2024
Department of Chemistry, Tsinghua University, Beijing 100084, People's Republic of China.
Oxygen evolution reaction (OER) is the pivotal obstacle of water splitting for hydrogen production. Dual-sites catalysts (DSCs) are considered exceeding single-site catalysts due to the preternatural synergetic effects of two metals in OER. However, appointing the specific spatial configuration of dual-sites toward more efficient catalysis still remains a challenge.
View Article and Find Full Text PDFACS Appl Mater Interfaces
December 2023
Institute of Materials Research and Engineering (IMRE), A*STAR (Agency for Science, Technology and Research), 2 Fusionopolis Way, Innovis, #08-03138634 ,Republic of Singapore.
Atomically dispersed single-atom catalysts are intriguing catalysts in the field of electrocatalysis for nearly 100% exploitation of metal atoms. However, they are still far from practical usage due to the scaling relationship limit and metal loading limit. Generation of a diatomic complex would offer superior catalytic performance through the cooperation of two neighboring atoms as active sites.
View Article and Find Full Text PDFACS Omega
June 2023
School of Environment, Tsinghua University, Beijing 10084, China.
Catalytic ozonation is an effective and promising advanced oxidation technology for organic pollutant removal. Herein, CexMnO metal oxides loaded on AlO catalysts (Mn-Ce/AlO) were synthesized for catalytic ozonation of the wastewater containing ciprofloxacin. The morphology, crystal structure, and specific surface area of the prepared catalyst were characterized.
View Article and Find Full Text PDFAdv Sci (Weinh)
August 2023
State Key Laboratory of Food Science and Resources, School of Food Science and Technology, Jiangnan University, Wuxi, Jiangsu, 214122, P. R. China.
Designing and synthesizing advanced electrocatalysts with superior intrinsic activity toward hydrogen evolution reaction (HER) in alkaline media is critical for the hydrogen economy. Herein, a novel Ir@Rhene heterojunction electrocatalyst is synthesized via epitaxially confining ultrasmall and low-coordinate Ir nanoclusters on the ultrathin Rh metallene accompanying the formation of Ir/IrO Janus nanoparticles. The as-prepared heterojunctions display outstanding alkaline HER activity, with an overpotential of only 17 mV at 10 mA cm and an ultralow Tafel slope of 14.
View Article and Find Full Text PDFAdv Mater
January 2023
The University of Sydney, School of Chemical and Biomolecular Engineering, Sydney, New South Wales, 2006, Australia.
Room-temperature sodium-sulfur (RT-Na/S) batteries possess high potential for grid-scale stationary energy storage due to their low cost and high energy density. However, the issues arising from the low S mass loading and poor cycling stability caused by the shuttle effect of polysulfides seriously limit their operating capacity and cycling capability. Herein, sulfur-doped graphene frameworks supporting atomically dispersed 2H-MoS and Mo (S@MoS -Mo /SGF) with a record high sulfur mass loading of 80.
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