High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials
Zhiyi Lu,Guangxu Chen,Samira Siahrostami,Zhihua Chen,Kai Liu,Jin Xie,Lei Liao,Tong Wu,Dingchang Lin,Yayuan Liu,Thomas F. Jaramillo,Jens K. Nørskov,Jens K. Nørskov,Yi Cui,Yi Cui +14 more
- Vol. 1, Iss: 2, pp 156-162
TLDR
In this article, a facile and general approach to catalyst development via surface oxidation of abundant carbon materials to significantly enhance both the activity and selectivity for H2O2 production by electrochemical oxygen reduction was demonstrated.Abstract:
Hydrogen peroxide (H2O2) is a valuable chemical with a wide range of applications, but the current industrial synthesis of H2O2 involves an energy-intensive anthraquinone process. The electrochemical synthesis of H2O2 from oxygen reduction offers an alternative route for on-site applications; the efficiency of this process depends greatly on identifying cost-effective catalysts with high activity and selectivity. Here, we demonstrate a facile and general approach to catalyst development via the surface oxidation of abundant carbon materials to significantly enhance both the activity and selectivity (~90%) for H2O2 production by electrochemical oxygen reduction. We find that both the activity and selectivity are positively correlated with the oxygen content of the catalysts. The density functional theory calculations demonstrate that the carbon atoms adjacent to several oxygen functional groups (–COOH and C–O–C) are the active sites for oxygen reduction reaction via the two-electron pathway, which are further supported by a series of control experiments. The direct synthesis of hydrogen peroxide via oxygen reduction is an attractive alternative to the anthraquinone process. Here, a general trend linking oxygenation of carbon surfaces with electrocatalytic performance in peroxide synthesis is demonstrated, and computational studies provide further insight into the nature of the active sites.read more
Citations
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High-entropy ceramics
TL;DR: In this paper, the authors discuss the current state of the disordered ceramics field by examining the applications and the high-entropy features fuelling them, covering both theoretical predictions and experimental results.
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Isolated Diatomic Ni-Fe Metal-Nitrogen Sites for Synergistic Electroreduction of CO2.
TL;DR: Density functional theory studies reveal that the neighboring Ni-Fe centers not only function in synergy to decrease the reaction barrier for the formation of COOH* and desorption of CO, but also undergo distinct structural evolution into a CO-adsorbed moiety upon CO2 uptake.
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Atomic-level tuning of Co-N-C catalyst for high-performance electrochemical H2O2 production.
Euiyeon Jung,Heejong Shin,Byounghoon Lee,Vladimir Efremov,S. H. Lee,Hyeon Seok Lee,Jiheon Kim,Wytse Hooch Antink,Subin Park,Kug-Seung Lee,Sung-Pyo Cho,Jong Suk Yoo,Yung-Eun Sung,Taeghwan Hyeon +13 more
TL;DR: Interestingly, guided by first-principles calculations, it is found that the catalytic properties of the Co–N4 moiety can be tailored by fine-tuning its surrounding atomic configuration to resemble the structure-dependent catalytic Properties of metalloenzymes.
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Edge-Site Engineering of Atomically Dispersed Fe-N4 by Selective C-N Bond Cleavage for Enhanced Oxygen Reduction Reaction Activities.
TL;DR: Both experiments and theoretical calculations verified the selective C-N bond cleavage adjacent to Fe center induced by porosity engineering could form edge-hosted Fe-N4 moieties, and therefore lower the overall oxygen reduction reaction barriers comparing to intact atomic configuration.
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Atomic site electrocatalysts for water splitting, oxygen reduction and selective oxidation.
TL;DR: This review presents a systematic review on the fabrication routes of ASCs followed by an overview of some new and effective characterization methods to precisely probe the atomic structure and discusses the challenges and opportunities on the further development of more selective, active, stable and less expensive ASCs.
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Chemical oxidation of multiwalled carbon nanotubes
Vitaliy Datsyuk,M. Kalyva,Konstantinos Papagelis,John Parthenios,Dimitrios Tasis,Angeliki Siokou,Ioannis Kallitsis,Costas Galiotis +7 more
TL;DR: In this article, the effect of oxidation on the structural integrity of multiwalled carbon nanotubes through acidic (nitric acid and a mixture of sulfuric acid and hydrogen peroxide) and basic (ammonium hydroxide/hydrogen peroxide), agents has been studied.