ABSTRACT
Providing affordable safe drinking water and universal sanitation poses a grand challenge especially after the global COVID-19 pandemic. In this work, we developed atomically dispersed Au on potassium-incorporated polymeric carbon nitride (AuKPCN) that could simultaneously boost photocatalytic generation of ·OH and H2O2 with an apparent quantum efficiency over 90% at 400–420 nm. The introduction of potassium into the poly(heptazine imide) matrix formed strong K-N bonds, preventing Au from forming strong interactions with N. Instead, Au formed a bond with C, only having weak interactions with N on KPCN, which rendered Au with an oxidation number close to 0. The results of in-situ vibrational spectroscopy, isotopic experiments, transient absorption spectroscopy and time-dependent density functional theory (TDDFT) simulations revealed that the low-valent Au could append its 6s orbital into the band diagram of AuKPCN that formed a trapping level for generating highly localized holes under photoexcitation. These highly localized holes could boost the 1e− water oxidation reaction to form highly oxidative ·OH and simultaneously unbind the hydrogen atom in H2O molecule, which greatly promoted the hydrogenation process during the 2e− oxygen reduction reaction (ORR) to produce H2O2. The photogenerated ·OH on AuKPCN led to a more than 120-fold efficiency enhancement for visible-light-response superhydrophilicity as compared to that of the commercial TiO2. The onsite fixed-bed reactor under photo-illumination achieved a remarkable 132.5 LH2O m− 2 day− 1 water disinfection rate (lg6), which is about 30 times superior than the TiO2 photocatalytic advanced oxidation process in the most ideal case (< 4 LH2O m− 2 day− 1; lg4).
Subject(s)
COVID-19ABSTRACT
Aerosol particles originated from anthropogenic emissions, volcanic eruptions, biomass burning, and fossil combustion emissions, and their radiative effect is one of the most uncertain factors in climate change. Meanwhile, aerosol particles in fine particle size could also cause irreversible effects on the human respiratory system. This study attempted to analyse the spatial and temporal variations of global aerosol optical depth (AOD, 550 nm) during 1980–2018 using MERRA-2 aerosol reanalysis products and to investigate the effects of natural/anthropogenic emissions of different types of aerosols on AOD values. The results show that the global annual mean AOD values kept high levels with significant fluctuations during 1980–1995 and showed a consistent decreasing and less volatile trend after 1995. Spatially, the AOD values are relatively higher in the Northern Hemisphere than in the Southern Hemisphere, especially in North Africa (0.329), Northern India (0.235), and Eastern China (0.347), because of the intensive natural/anthropogenic aerosol emissions there. The sulphate-based aerosols emitted by biomass burning and anthropogenic emissions are the main types of aerosols worldwide, especially in densely populated and industrialized regions such as East Asia and Europe. Dust aerosols are also the main aerosol type in desert areas. For example, the AOD and AODP values for the Sahara Desert are 0.3178 and 75.32%, respectively. Both black carbon aerosols (BC) and organic carbon aerosols (OC) are primary or secondary from carbon emissions of fossil fuels, biomass burning, and open burning. Thus, the regions with high BC and OC aerosol loadings are mainly located in densely populated or vegetated areas such as East Asia, South Asia, and Central Africa. Sea salt aerosols are mainly found in coastline areas along the warm current pathway. This study could help relevant researchers in the fields of atmospheric science, environmental protection, air pollution, and ecological environment to understand the global spatial–temporal variations and main driving factors of aerosol loadings.