Developing highly efficient, cost-effective, and robust electrocatalysts for the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) is paramount for the large-scale commercialization of renewable fuel cells and rechargeable metal-air batteries. Herein, a new ternary-atom catalyst that is composed of paired Fe sites and single Ni sites (as Fe-N and Ni-N) coordinated onto hollow nitrogen-doped carbon microspheres is developed. The as-synthesized catalyst exhibits remarkable activities toward both the ORR and OER in alkaline media, with superior performances to those of the control materials that contain only Fe-N or Ni-N sites. Density functional theory calculations and in situ infrared (IR) spectroscopic studies clearly reveal that the Fe-N centers are the active sites for both ORR and OER, and their electrocatalytic activities are synergistically enhanced through optimization of their d-band centers by the Ni-N sites. This ternary-atom catalyst can potentially be a promising, alternative, sustainable catalyst to commercially used Pt- and Ru-based catalysts to drive both the ORR and the OER in rechargeable zinc-air batteries and other related applications.
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http://dx.doi.org/10.1002/anie.202421168 | DOI Listing |
Chemistry
December 2024
YUAN ZE UNIVERSITY, DEPARTMENT OF CHEMICAL ENGINEERING AND MATERIALS SCIENCE, YUAN-TUNG RD., 320, TAOYUAN, TAIWAN.
Nano-sized high-entropy materials (HEMs) recently received more attention to researchers due to their superior electrochemical catalytic properties. HEMs comprise at least five elements with or without metals and are synthesized through solid-state reactions and solution-mediated techniques. The presence of many elements in these HEMs result in a high mixing entropy and facilitates the formation of stable solid solutions in fundamental crystal structures.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Hunan University, College of Chemistry and Chemical Engineering, No.2 Lushan Southroad, 410000, Changsha, CHINA.
Mimicking natural enzymes through artificial enzyme engineering represents a powerful strategy to fine-tune the performance of photocatalysts, while the manipulation of electron transfer systems through atomic precision control is challenging. Herein, we reported a series of covalent organic frameworks (COFs) based on progressively oxidized phenothiazine (PTH) core as the platform for emulating Coenzyme Q, achieved through meticulous stepwise adjustments of their redox states. Compared to the original PTH-S-COF, the COFs with incrementally oxidized sulfur sites exhibited enhanced charge transfer efficiencies, facilitating efficient electron donation to O2 and thereby providing a favorable pathway for H2O2 synthesis.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Tsinghua University, Zhongguancun North Street, Haidian District, 100084, BEIJING, CHINA.
The rational design of metal oxide catalysts with enhanced oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) performance is crucial for the practical application of aqueous rechargeable zinc-air batteries (a-r-ZABs). Precisely regulating the electronic environment of metal-oxygen (M-O) active species is critical yet challenging for improving their activity and stability toward OER and ORR. Herein, we propose an atomic-level bilateral regulation strategy by introducing atomically dispersed Ga for continuously tuning the electronic environment of Ru-O and Mn-O in the Ga/MnRuO2 catalyst.
View Article and Find Full Text PDFNanoscale Adv
December 2024
Department of Biomedical Engineering, Faculty of Engineering and Natural Sciences, Istinye University Istanbul 34396 Turkiye
Recently, interest has surged in the environmental and biomedical applications of two-dimensional transition metal borides, commonly referred to as MBenes. These materials have emerged as promising candidates for energy storage devices, such as batteries and supercapacitors. Additionally, MBenes have shown remarkable catalytic activity due to their high surface area and tunable electronic properties.
View Article and Find Full Text PDFJ Colloid Interface Sci
December 2024
College of Urban and Environmental Sciences, Huangshi Key Laboratory of Prevention and Control of Soil Pollution, Hubei Normal University, Huangshi 435002, PR China. Electronic address:
The development of carbon-encapsulated alloy catalysts, through a rational design that integrates highly active Me-N-C sites, is essential for improving the reaction kinetics of both oxygen reduction (ORR) and oxygen evolution reactions (OER). This advancement is pivotal for the progression of efficient rechargeable zinc-air batteries (RZABs). In this study, we investigates a CoNi alloy decorated N-doped carbon nanotube (CoNi-NCNT) electrocatalyst using a dual-ligand strategy.
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