Single‐atom catalysts have emerged as an efficient oxidant activator for eliminating organic pollutants in Fenton‐like systems. However, the complex preparation, single active site, lack of ...understanding of the fundamental mechanism, and harsh pH conditions currently limit their practical applications. In this work, single‐atom iron anchored nitrogen‐rich g‐C3N4 nanotubes (FeCNs) are designed and synthesized by a facile approach, and eco‐friendly peracetic acid (PAA) is selected as the oxidant for Fenton‐like reactions. The constructed heterogenous system achieves an enhanced degradation of various organic contaminants over a wide pH range of 3.0–9.0, exhibiting an ultrahigh and stable catalytic activity, outperforming equivalent quantities of pristine g‐C3N4 by 75 times. The 18O isotope‐labeling technique, probe method, and theoretical calculations demonstrate that the efficient catalytic activity relies on the high‐valency iron‐oxo species coupled with organic radicals generated by PAA. An increase in electron transport from the contaminant to the formed “metastable PAA/FeCN catalyst surface complex” is detected. A double driving mechanism for the tubular g‐C3N4 regulated by a single Fe site and PAA activation is proposed. This work opens an avenue for developing novel catalysts with the coexistence of multiple active units and providing opportunities for significantly improving catalytic efficiency.
Atomically dispersing Fe(III) sites into fine‐tuned nitrogen‐rich graphitic carbon nitride nanotubes are designed for peracetic acid activation and further for Fenton‐like reactions. This work opens a new avenue to develop heterogenous catalytic systems with higher reactivity and better durability using a double engine mechanism.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
The construction of enzyme-inspired artificial catalysts with enzyme-like active sites and microenvironment remains a great challenge. Herein, we report a single-atomic-site Co catalyst supported by ...carbon doped boron nitride (BCN) with locally polarized B-N bonds (Co SAs/BCN) to simulate the reductive dehalogenases. Density functional theory analysis suggests that the BCN supports, featured with ionic characteristics, provide additional electric field effect compared with graphitic carbon or N-doped carbon (CN), which could facilitate the adsorption of polarized organochlorides. Consistent with the theoretical results, the Co SAs/BCN catalyst delivers a high activity with nearly complete dechlorination (~98%) at a potential of -0.9 V versus Ag/AgCl for chloramphenicol (CAP), showing that the rate constant (k) contributed by unit mass of metal (k/ratio) is 4 and 19 times more active than those of the Co SAs/CN and state-of-the-art Pd/C catalyst, respectively. We show that Co single atoms coupled with BCN host exhibit high stability and selectivity in CAP dechlorination and suppress the competing hydrogen evolution reaction, endowing the Co SAs/BCN as a candidate for sustainable conversion of organic chloride.
The development of high‐efficiency bifunctional electrocatalyst for oxygen reduction and evolution reactions (ORR/OER) is critical for rechargeable metal–air batteries, a typical electrochemical ...energy storage and conversion technology. This work reports a general approach for the synthesis of Pd@PdO–Co3O4 nanocubes using the zeolite‐type metal–organic framework (MOF) as a template. The as‐synthesized materials exhibit a high electrocatalytic activity toward OER and ORR, which is comparable to those of commercial RuO2 and Pt/C electrocatalysts, while its cycle performance and stability are much higher than those of commercial RuO2 and Pt/C electrocatalysts. Various physicochemical characterizations and density functional theory calculations indicate that the favorable electrochemical performance of the Pd@PdO–Co3O4 nanocubes is mainly attributed to the synergistic effect between PdO and the robust hollow structure composed of interconnected crystalline Co3O4 nanocubes. This work establishes an efficient approach for the controlled design and synthesis of MOF‐templated hybrid nanomaterials, and provides a great potential for developing high‐performance electrocatalysts in energy storage and conversion.
This work reports a general approach to synthesize Pd@PdO‐Co3O4 nanocubes using the zeolite‐type metal–organic framework (MOF) as a template. The as‐synthesized material exhibits a high electrocatalytic activity toward Oxygen evolution and reduction reactions (OER and ORR). Synergistic effects between PdO and the robust hollow structure crystalline Co3O4 nanocubes are the main contributions to the catalyst's excellent performance.
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FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Removal of organic micropollutants from water through advanced oxidation processes (AOPs) is hampered by the excessive input of energy and/or chemicals as well as the large amounts of residuals ...resulting from incomplete mineralization. Herein, we report a new water purification paradigm, the direct oxidative transfer process (DOTP), which enables complete, highly efficient decontamination at very low dosage of oxidants. DOTP differs fundamentally from AOPs and adsorption in its pollutant removal behavior and mechanisms. In DOTP, the nanocatalyst can interact with persulfate to activate the pollutants by lowering their reductive potential energy, which triggers a non-decomposing oxidative transfer of pollutants from the bulk solution to the nanocatalyst surface. By leveraging the activation, stabilization, and accumulation functions of the heterogeneous catalyst, the DOTP can occur spontaneously on the nanocatalyst surface to enable complete removal of pollutants. The process is found to occur for diverse pollutants, oxidants, and nanocatalysts, including various low-cost catalysts. Significantly, DOTP requires no external energy input, has low oxidant consumption, produces no residual byproducts, and performs robustly in real environmental matrices. These favorable features render DOTP an extremely promising nanotechnology platform for water purification.
The sparse representation of a multiple-measurement vector (MMV) is a relatively new problem in sparse representation. Efficient methods have been proposed. Although many theoretical results that are ...available in a simple case-single-measurement vector (SMV)-the theoretical analysis regarding MMV is lacking. In this paper, some known results of SMV are generalized to MMV. Some of these new results take advantages of additional information in the formulation of MMV. We consider the uniqueness under both an lscr 0 -norm-like criterion and an lscr 1 -norm-like criterion. The consequent equivalence between the lscr 0 -norm approach and the lscr 1 -norm approach indicates a computationally efficient way of finding the sparsest representation in a redundant dictionary. For greedy algorithms, it is proven that under certain conditions, orthogonal matching pursuit (OMP) can find the sparsest representation of an MMV with computational efficiency, just like in SMV. Simulations show that the predictions made by the proved theorems tend to be very conservative; this is consistent with some recent advances in probabilistic analysis based on random matrix theory. The connections will be discussed
•Long-term exposure to PM2.5 and/or PM10 is associated with increased mortality.•Associations with PM2.5 were more consistent than with PM10.•Associations with PM2.5 remained at low exposure levels.
...As new scientific evidence on health effects of air pollution is generated, air quality guidelines need to be periodically updated. The objective of this review is to support the derivation of updated guidelines by the World Health Organization (WHO) by performing a systematic review of evidence of associations between long-term exposure to particulate matter with diameter under 2.5 µm (PM2.5) and particulate matter with diameter under 10 µm (PM10), in relation to all-cause and cause-specific mortality. As there is especially uncertainty about the relationship at the low and high end of the exposure range, the review needed to provide an indication of the shape of the concentration–response function (CRF).
We systematically searched MEDLINE and EMBASE from database inception to 9 October 2018. Articles were checked for eligibility by two reviewers. We included cohort and case-control studies on outdoor air pollution in human populations using individual level data. In addition to natural-cause mortality, we evaluated mortality from circulatory diseases (ischemic heart disease (IHD) and cerebrovascular disease (stroke) also specifically), respiratory diseases (Chronic Obstructive Pulmonary Disease (COPD) and acute lower respiratory infection (ALRI) also specifically) and lung cancer. A random-effect meta-analysis was performed when at least three studies were available for a specific exposure-outcome pair. Risk of bias was assessed for all included articles using a specifically developed tool coordinated by WHO. Additional analyses were performed to assess consistency across geographic region, explain heterogeneity and explore the shape of the CRF. An adapted GRADE (Grading of Recommendations Assessment, Development and Evaluation) assessment of the body of evidence was made using a specifically developed tool coordinated by WHO.
A large number (N = 107) of predominantly cohort studies (N = 104) were included after screening more than 3000 abstracts. Studies were conducted globally with the majority of studies from North America (N = 62) and Europe (N = 25). More studies used PM2.5 (N = 71) as the exposure metric than PM10 (N = 42). PM2.5 was significantly associated with all causes of death evaluated. The combined Risk Ratio (RR) for PM2.5 and natural-cause mortality was 1.08 (95%CI 1.06, 1.09) per 10 µg/m3. Meta analyses of studies conducted at the low mean PM2.5 levels (<25, 20, 15, 12, 10 µg/m3) yielded RRs that were similar or higher compared to the overall RR, consistent with the finding of generally linear or supra-linear CRFs in individual studies. Pooled RRs were almost identical for studies conducted in North America, Europe and Western Pacific region. PM10 was significantly associated with natural-cause and most but not all causes of death. Application of the risk of bias tool showed that few studies were at a high risk of bias in any domain. Application of the adapted GRADE tool resulted in an assessment of “high certainty of evidence” for PM2.5 with all assessed endpoints except for respiratory mortality (moderate). The evidence was rated as less certain for PM10 and cause-specific mortality (“moderate” for circulatory, IHD, COPD and “low” for stroke mortality.
Compared to the previous global WHO evaluation, the evidence base has increased substantially. However, studies conducted in low- and middle- income countries (LMICs) are still limited. There is clear evidence that both PM2.5 and PM10 were associated with increased mortality from all causes, cardiovascular disease, respiratory disease and lung cancer. Associations remained below the current WHO guideline exposure level of 10 µg/m3 for PM2.5.
Systematic review registration number (PROSPERO ID): CRD42018082577.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
Internet has made the communication environment of ideological and political education (IPE) more complex for university students. Therefore, it is necessary to investigate the impact of university ...students' Internet literacy and contact on the communication effects of IPE.
A total of 2283 Chinese university students were recruited to complete verified online questionnaires on Internet literacy, Internet contact duration, and the communication effects of IPE. SPSS V20 statistical software was used for the ordinal logistic regression analysis, chi-square test, and t-test.
Up to 95.31 % of the university students obtained information through the Internet. There were significant differences between the ILS-high (54.93 %) and ILS-low (45.07 %) groups in both Internet literacy (P < 0.001) and Internet contact (P < 0.001). When comparing the communication effects of IPE between the ILS-high and ILS-low groups, both groups had the best emotional items and the worst cognitive dimensions. Internet literacy, Internet contact, major, and gender significantly impacted the communication effects of IPE.
In the Internet era, there is an urgent need to improve university students' Internet literacy, so that they can have high Internet self-control contact skills to give full play to the positive guiding role of network media and improve the communication effects of university students' IPE.
•Up to 95.31% university students obtained information through the Internet.•There were significant differences between ILS-high and ILS-low group in Internet literacy and Internet contact.•Both ILS-high and ILS-low groups showed the best emotional and the worst cognitive communication effect of IPE.•Internet literacy and Internet contact had significant impacts on communication effects of IPE.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
Due to their biocompatibility and non-toxic nature, biomedical polymer materials have found widespread applications and significantly propelled the progress of the biomedical field ....
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IZUM, KILJ, NUK, PILJ, PNG, SAZU, UL, UM, UPUK
To feed its 1.3 billion population with a per capita cultivated land far below the world average, China is already facing a great challenge of land scarcity. Accelerated urbanization along with ...explosive economic growth has further worsened the shortage of agricultural land over the last two decades. Increasing concern over land is expressed in terms of soil availability for grain production and soil quality degradation. Based on official statistics and data derived from satellite imagery, dynamics of China's cultivated land over the past two decades is outlined and the causes and destinations of cultivated land loss are analyzed in this paper. Particularly, urbanization-related land-use changes and their spatial variation across the country are demonstrated. Furthermore, impacts of urbanization and associated waste disposals, consequent shifts of soil utilization on areal soil quality are expatiated. It is initially concluded that China's cultivated land is shrinking at a rather shocking rate. Although conversion to urban and industrial uses took up a comparatively small share of total cultivated land loss, urbanization should still be considered as a great threat to future agricultural production for several reasons. Urbanization is increasing the risk of soil pollution through waste disposal and acid deposition derived from urban air pollution. Facing rapid urbanization, China is making positive policy responses to the challenge of decreasing availability of cultivated land and offering unremitting efforts towards the goal of national food security.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
Interfacial electron transfer (IET) is essential for chemical and biological transformation of pollutants, operative across diverse lengths and time scales. This Perspective presents an array of ...multiscale molecular simulation methodologies, supplemented by in situ monitoring and imaging techniques, serving as robust tools to decode IET enhancement mechanisms such as interface molecular modification, catalyst coordination mode, and atomic composition regulation. In addition, three IET-based pollutant transformation systems, an electrocatalytic oxidation system, a bioelectrochemical spatial coupling system, and an enzyme-inspired electrocatalytic system, were developed, demonstrating a high effect in transforming and degrading pollutants. To improve the effectiveness and scalability of IET-based strategies, the refinement of these systems is necessitated through rigorous research and theoretical exploration, particularly in the context of practical wastewater treatment scenarios. Future endeavors aim to elucidate the synergy between biological and chemical modules, edit the environmental functional microorganisms, and harness machine learning for designing advanced environmental catalysts to boost efficiency. This Perspective highlights the powerful potential of IET-focused environmental remediation strategies, emphasizing the critical role of interdisciplinary research in addressing the urgent global challenge of water pollution.
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