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null (Ed.)Abstract Developing efficient and stable earth-abundant electrocatalysts for acidic oxygen evolution reaction is the bottleneck for water splitting using proton exchange membrane electrolyzers. Here, we show that nanocrystalline CeO 2 in a Co 3 O 4 /CeO 2 nanocomposite can modify the redox properties of Co 3 O 4 and enhances its intrinsic oxygen evolution reaction activity, and combine electrochemical and structural characterizations including kinetic isotope effect, pH- and temperature-dependence, in situ Raman and ex situ X-ray absorption spectroscopy analyses to understand the origin. The local bonding environment of Co 3 O 4 can be modified after the introduction of nanocrystalline CeO 2 , which allows the Co III species to be easily oxidized into catalytically active Co IV species, bypassing the potential-determining surface reconstruction process. Co 3 O 4 /CeO 2 displays a comparable stability to Co 3 O 4 thus breaks the activity/stability tradeoff. This work not only establishes an efficient earth-abundant catalysts for acidic oxygen evolution reaction, but also provides strategies for designing more active catalysts for other reactions.
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Electrochemical synthesis of hydrogen peroxide (H 2 O 2 ) in acidic solution can enable the electro-Fenton process for decentralized environmental remediation, but robust and inexpensive electrocatalysts for the selective two-electron oxygen reduction reaction (2e − ORR) are lacking. Here, we present a joint computational/experimental study that shows both structural polymorphs of earth-abundant cobalt diselenide (orthorhombic o -CoSe 2 and cubic c -CoSe 2 ) are stable against surface oxidation and catalyst leaching due to the weak O* binding to Se sites, are highly active and selective for the 2e − ORR, and deliver higher kinetic current densities for H 2 O 2 production than the state-of-the-art noble metal or single-atom catalysts in acidic solution. o -CoSe 2 nanowires directly grown on carbon paper electrodes allow for the steady bulk electrosynthesis of H 2 O 2 in 0.05 M H 2 SO 4 with a practically useful accumulated concentration of 547 ppm, the highest among the reported 2e − ORR catalysts in acidic solution. Such efficient and stable H 2 O 2 electrogeneration further enables the effective electro-Fenton process for model organic pollutant degradation.
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A reliable projection of future South Asian summer monsoon (SASM) benefits a large population in Asia. Using a 100-member ensemble of simulations by the Max Planck Institute Earth System Model (MPI-ESM) and a 50-member ensemble of simulations by the Canadian Earth System Model (CanESM2), we find that internal variability can overshadow the forced SASM rainfall trend, leading to large projection uncertainties for the next 15 to 30 years. We further identify that the Interdecadal Pacific Oscillation (IPO) is, in part, responsible for the uncertainties. Removing the IPO-related rainfall variations reduces the uncertainties in the near-term projection of the SASM rainfall by 13 to 15% and 26 to 30% in the MPI-ESM and CanESM2 ensembles, respectively. Our results demonstrate that the uncertainties in near-term projections of the SASM rainfall can be reduced by improving prediction of near-future IPO and other internal modes of climate variability.