We investigated the role of Cu(II) ions and their associated structural features, such as chemical state and environment, in the Cu(II)-grafted TiO2 photocatalyst by means of 2-propanol oxidative decomposition under visible light and X-ray absorption fine structure (XAFS) measurements. The 2-propanol decomposition activity under visible light (1 mW cm−2, 450−580 nm) was highly reproducible (three repetitions). The XAFS results indicated that the Cu(II) is incorporated in a distorted amorphous CuO-like structure, having a five-coordinated square pyramidal form. The distorted CuO formed clusters and attached to the TiO2 surface. The chemical state and environment of the Cu(II) ions were not changed, even after the photocatalytic oxidative reaction. Thus, Cu(II)-grafted TiO2 can be regarded as a stable photocatalyst. In addition, in situ XAFS measurements were performed under visible light in the presence of 2-propanol and absence of oxygen. Under these conditions, Cu(I) was generated. However, the latter converted back to Cu(II) when it was exposed to oxygen, indicating the oxygen reduction activity of Cu(I).
We carried out in operando Mo K-edge X-ray absorption fine structure measurements on the rechargeable molecular cluster batteries (MCBs) of polyoxometalates (POMs), in which a Keggin-type POM, [PMo(12)O(40)](3-), is utilized as a cathode active material with a lithium metal anode. The POM-MCBs exhibit a large capacity of ca. 270 (A h)/kg in a voltage range between V = 4.0 V and V = 1.5 V. X-ray absorption near-edge structure analyses demonstrate that all 12 Mo(6+) ions in [PMo(12)O(40)](3-) are reduced to Mo(4+) in the discharging process. This means the formation of a super-reduced state of the POM, namely, [PMo(12)O(40)](27-), which stores 24 electrons, and this electron number can explain the large capacity of the POM-MCBs. Furthermore, extended X-ray absorption fine structure analyses reveal the molecular structure of [PMo(12)O(40)](27-), which is slightly reduced in size compared to the original [PMo(12)O(40)](3-) and involves Mo(4+) metal-metal-bonded triangles. Density functional theory calculations suggest that these triangles are formed because of the large number of additional electrons in the super-reduced state.
The adsorption structure of methylthiolate (CH3S) adsorbed on Au(111), a long-standing controversial issue, has been unambiguously determined by scanned-energy and scanned-angle S 2p photoelectron diffraction. The methylthiolate molecules are found to occupy atop sites with a S-Au distance of 2.42 +/- 0.03 A. The angular distribution of the S 2p photoelectrons due to forward scattering reveals that the S-C bond is inclined by approximately 50 degrees from the surface normal towards both the [211] and [121] (nearest-neighbor thiolate) directions.
Favipiravir is an oral broad-spectrum inhibitor of viral RNA-dependent RNA polymerase that is approved for treatment of influenza in Japan. We conducted a prospective, randomized, open-label, multicenter trial of favipiravir for the treatment of COVID-19 at 25 hospitals across Japan. Eligible patients were adolescents and adults admitted with COVID-19 who were asymptomatic or mildly ill and had an Eastern Cooperative Oncology Group (ECOG) performance status of 0 or 1. Patients were randomly assigned at a 1:1 ratio to early or late favipiravir therapy (the same regimen starting on day 6 instead of day 1). The primary endpoint was viral clearance by day 6. The secondary endpoint was change in viral load by day 6. Exploratory endpoints included time to defervescence and resolution of symptoms. Eighty-nine patients were enrolled, of whom 69 were virologically evaluable. Viral clearance occurred within 6 days in 66.7% and 56.1% of the early and late treatment groups (adjusted hazard ratio [aHR], 1.42; 95% confidence interval [95% CI], 0.76–2.62). Of 30 patients who had a fever (≥37.5°C) on day 1, time to defervescence was 2.1 days and 3.2 days in the early and late treatment groups (aHR, 1.88; 95%CI, 0.81–4.35). During therapy, 84.1% developed transient hyperuricemia. Favipiravir did not significantly improve viral clearance as measured by RT-PCR by day 6 but was associated with numerical reduction in time to defervescence. Neither disease progression nor death occurred to any of the patients in either treatment group during the 28-day participation (Japan Registry of Clinical Trials jRCTs041190120).
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