Molecular
hydrogen is one of the essential reactants in the chemical
industry, and its generation from renewable sources such as biomass
materials and water is of great benefit to the future society. Generally,
molecular oxygen should be pre-eliminated in the hydrogen evolution
reactions (HERs) in order to avoid the reverse hydrogen oxidation
reaction (HOR). Here, we report a highly efficient HER from a formaldehyde/water
mixture using MgO supported Ag nanoparticles (AgNPs/MgO) as the catalyst
and molecular oxygen as a promoter. The HER rate depends almost linearly
on the oxygen partial pressure, and the optimal turnover frequency
(TOF) of the silver catalyst exceeds 6,600 h–1.
Based on the experimental and theoretical results, a surface stabilized
MgO/Ag–•OOH complex is suggested to be the
main catalytically active species for the HER.
We show here the first radical route for the direct photosynthesis of AuCN oligomers with different sizes and shapes, as evidenced by TEM observations, from an Au nanoparticle/benzaldehyde/CH(3)CN ternary system in air under UV-light irradiation. This photochemical route is green, mild, and universal, which makes itself distinguishable from the common cyanidation process. Several elementary reaction steps, including the strong C-C bond dissociation of CH(3)CN and subsequent •CN radical addition to Au, have been suggested to be critical in the formation of AuCN oligomers based on the identification of •CN radical by in situ EPR and the radical trapping technique, and other reaction products by GC-MS and (1)H NMR, and DFT calculations. The resulting solid-state AuCN oligomers exhibit unique spectroscopic characters that may be a result of the shorter Au-Au distances (namely, aurophilicity) and/or special polymer-like structures as compared with gold cyanide derivatives in the aqueous phase. The nanosized AuCN oligomers supported on mesoporous silica showed relatively good catalytic activity on the homogeneous annulation of salicylaldehyde with phenylacetylene to afford isoflavanones employing PBu(3) as the cocatalyst under moderate conditions, which also serves as evidence for the successful production of AuCN oligomers.
In order to understand the influence of nitrogen (N) deposition on the key processes relevant to the carbon (C) balance in a bamboo plantation, a twoyear field experiment involving the simulated deposition of N in a Pleioblastus amarus plantation was conducted in the rainy region of SW China. Four levels of N treatments: control (no N added), low-N (50 kg N ha −1 year −1 ), medium-N (150 kg N ha −1 year −1 ), and high-N (300 kg N ha −1 year −1 ) were set in the present study. The results showed that soil respiration followed a clear seasonal pattern, with the maximum rates in mid-summer and the minimum in late winter. The annual cumulative soil respiration was 585±43 g CO 2 -C m −2 year −1 in the control plots. Simulated N deposition significantly increased the mean annual soil respiration rate, fine root biomass, soil microbial biomass C (MBC), and N concentration in fine roots and fresh leaf litter. Soil respirations exhibited a positive exponential relationship with soil temperature, and a linear relationship with MBC. The net primary production (NPP) ranged from 10.95 to 15.01 Mg C ha −1 year −1 and was higher than the annual soil respiration (5.85 to 7.62 Mg C ha −1 year −1 ) in all treatments. Simulated N deposition increased the net ecosystem production (NEP), and there was a significant difference between the control and high N treatment NEP, whereas, the difference of NEP among control, low-N, and medium-N was not significant. Results suggest that N controlled the primary production in this bamboo plantation ecosystem. Simulated N deposition increased the C sequestration of the P. amarus plantation ecosystem through increasing the plant C pool, though CO 2 emission through soil respiration was also enhanced.
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