ABSTRACT:We here first proposed a yolk−shell Co 3 O 4 @ metal−organic frameworks (MOFs) nanoreactor via a facile method to accommodate sulfate radical-based advanced oxidation processes (SR-AOPs) into its interior cavity. The mesoporous and adsorptive MOFs shells allow the rapid diffusion of reactant molecules to the encapsulated Co 3 O 4 active sites, and the confined high instantaneous concentration of reactants in the local void space is anticipated to facilitate the SR-AOPs. As a proof of concept, the nanoreactor was fully characterized and applied for catalytic degradation of 4-chlorophenol (4-CP) in the presence of peroxymonosulfate (PMS). The enhancement of SR-AOPs in the nanoreactor is demonstrated by the result that degradation efficiency of 4-CP reached almost 100% within 60 min by using the yolk−shell Co 3 O 4 @MOFs catalysts as compared to only 59.6% under the same conditions for bare Co 3 O 4 NPs. Furthermore, the applicability of this nanoreactor used in SR-AOPs was systematically investigated in terms of effect of reaction parameters and identification of intermediates and primary radical as well as mineralization of the reaction and stability of the composite. The findings of this study elucidated a new opportunity for improved environmental remediation.

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[1] The Pacific Decadal Oscillation (PDO) has been shown to have significant climatic and environmental impacts across the Pan-Pacific Basin; however, there are no records of PDO activity from the South China Sea (SCS), the largest marginal sea in the northwest Pacific Ocean. This study suggests that a series of geochemical profiles obtained from a modern coral in the northern SCS records annual PDO activity dating back to 1853. These geochemical data are significantly correlated with the PDO index, and their patterns of variation closely match those of the PDO index over the last century. The relationship between the PDO and coral geochemistry may be related to the influence of the PDO on rainfall on Hainan Island. Rainfall patterns influence the volume of terrestrial runoff, which, in turn, is a primary determinant of

For the global oceans, the characteristics of high‐resolution climate changes during the last millennium remain uncertain because of the limited availability of proxy data. This study reconstructs climate conditions using annually resolved coral records from the South China Sea (SCS) to provide new insights into climate change over the last millennium. The results indicate that the climate of the Medieval Climate Anomaly (MCA, AD 900–1300) was similar to that of the Current Warm Period (CWP, AD 1850‐present), which contradicts previous studies. The similar warmth levels for the MCA and CWP have also been recorded in the Makassar Strait of Indonesia, which suggests that the MCA was not warmer than the CWP in the western Pacific and that this may not have been a globally uniform change. Hydrological conditions were drier/saltier during the MCA and similar to those of the CWP. The drier/saltier MCA and CWP in the western Pacific may be associated with the reduced precipitation caused by variations in the Pacific Walker Circulation. As for the Little Ice Age (LIA, AD 1550–1850), the results from this study, together with previous data from the Makassar Strait, indicate a cold and wet period compared with the CWP and the MCA in the western Pacific. The cold LIA period agrees with the timing of the Maunder sunspot minimum and is therefore associated with low solar activity. The fresher/wetter LIA in the western Pacific may have been caused by the synchronized retreat of both the East Asian Summer Monsoon and the Australian Monsoon.

Fe/Fe3C@N-doped porous carbon hybrids were synthesized as a robust and enhanced heterogeneous catalyst for peroxymonosulfate activation.

Long‐term seawater pH records are essential for evaluating the rates of ocean acidification (OA) driven by anthropogenic emissions. Widespread, natural decadal variability in seawater pH superimposes on the long‐term anthropogenic variations, likely influencing the OA rates estimated from the pH records. Here, we report a record of annual seawater pH estimated using the δ11B proxy over the past 159 years reconstructed from a Porites coral collected to the east of Hainan Island in the northern South China Sea (SCS). By coupling this time series with previously reported long‐term seawater pH records in the West Pacific, the decadal variability in seawater pH records and its possible driving mechanisms were investigated. The results indicate that large decadal variability in seawater pH has occurred off eastern Hainan Island over the past 159 years, in agreement with previous records. The Qiongdong upwelling system, which controls nutrient supplies, regulates surface water productivity, and is driven by the East Asian summer monsoon, is the primary control of this decadal variability, while terrestrial inputs appear not influence significantly. Meanwhile the impacts of the Pacific Decadal Oscillation (PDO) and the El Nino and Southern Oscillation (ENSO) systems on seawater pH off eastern Hainan Island is likely limited. In contrast, the PDO is the main factor to influence the decadal seawater pH variability offshore the East Australia, while the mechanism controlling the decadal seawater pH variability in Guam is not clear yet. Meanwhile, The rate of decrease in seawater pH estimated from coral records are significantly different in different regions and over different time spans, which may reflect a combination of natural decadal variability in seawater pH and long‐term variations. Therefore, understanding the mechanisms driving natural variability in seawater pH is important for improving estimates of ocean acidification rates driven by anthropogenic emissions.

Covalent triazine frameworks (CTFs) with high adsorption potential and photocatalytic ability features are expected to be designed as a new class of adsorbents that can regenerate themselves just by harnessing sunlight. To simultaneously improve both the adsorption and photocatalytic regeneration performance, a defect-abundant CTF-m was designed and tuned effectively by varying the lengths of benzene ring chains incorporated into the CTF backbone. It has been demonstrated that two kinds of defects in terms of broken benzene rings and pyrrole nitrogen were newly generated, other than the normal benzene rings and triazine units in the CTF-m skeleton. Benefiting from these defects, the adsorption sites with high energy for adsorbing volatile aromatic pollutants were significantly increased, which are reflected by higher saturated adsorption capacities of CTF-m (3.026 mmol/g for benzene (BEN), 1.490 mmol/g for naphthalene (NAP), and 0.863 mmol/g for phenol (PHE)) compared with those of CTF-1 and CTF-2. Furthermore, these defects narrowed the band structure and facilitated the separation of photogenerated charge carries, thus promoting photocatalytic regeneration. The percentage of CTF-m regenerated was still higher than 90% in the fourth cycle. These experimental results, together with the density functional theory (DFT) studies, soundly corroborated that the defects could optimize the adsorption and regeneration property of CTF-m. The present work highlights the potential of fabrication of defective CTFs as solar-driven self-cleaning adsorbents to remove pollutants from water.