1,694 pubs · 190,775 cites · h-index 228
Riverine and lake ecosystems are sources of global non-CO2 greenhouse gases (GHGs) and serve as sinks for pollutants, facing the dual challenges of mitigating GHG emissions and controlling water pollution. However, interactions between pollutant inputs and GHG emissions remain unclear. Herein, relying on a compiled data set of global non-CO2 GHGs and robust modeling, a watershed dissolved CH4 and N2O estimator is developed and validated on the global scale. Using the Dongting watershed (DTW) as a modeling example, various pollutant input scenarios were developed to explore the influence of changes in pollutant inputs on CO2-equivalent (CO2e) emissions from CH4 and N2O. Simulation results indicate that implementing pollutant inputs reduction measures in dissolved GHG hotspot areas will yield more efficient CO2e emission reduction benefits. Moreover, a critical paradox was revealed: while decreasing pollutant inputs leads to a sustained decline in direct CO2e (CO2eD) emissions, indirect CO2e (CO2eI) emissions from aquatic systems may show a minimal reduction in some cases. This paradox is closely tied to carbon–nitrogen ratio variations in aquatic system and can be well explained by carbon and nitrogen limitation principle, as defined by the Redfield ratio. Thus, our study suggests that cocontrol of carbon and nitrogen inputs within dissolved GHG hotspot areas is vital for achieving both water quality improvement and climate change mitigation simultaneously.
This framework improves execution accuracy in agent systems, suggesting effective tool-calling in enterprises.
Advanced oxidation processes (AOPs) by carbon-based single-atom catalysts (SACs) are recognized as an attractive scientific frontier for water treatment, with the outstanding benefits of ultra-effective and anti-interference capability. However, most of the research has paid more attention to the performance of SACs, while the in-depth understanding of catalytic regulation by molecular interaction is relatively deficient. This critical review delves into deciphering the catalytic mechanism through a micro-level, which makes it more convenient to interpret apparent catalytic phenomena. It first summarizes basic theories of quantum chemistry, which provide mechanism interpretation and prediction for molecular-oxidation systems. Additionally, corresponding oxidation pathways of common oxidants are underscored. Following the oxidants, state-of-the-art regulation methods are discussed with special attention to involved molecular interactions and pollutants. Particularly, the preliminary insights into the "oxidant-catalyst-pollutants" internal relationships are provided to help construct the SAC-AOP system from a molecular standpoint. Meanwhile, some cutting-edge laboratory devices and pilot-scale engineering are presented to illustrate the ultimate purpose of scientific molecular exploration. Eventually, relative challenges of SACs-AOPs upon the design of catalytic systems and investigation methods are provided. This review aims to promote the large-scale potential of SACs-based AOPs in practical water treatment by emphasizing the pivotal role of micro-insights.
Atom‐site catalysts, especially for graphitic carbon nitride‐based catalysts, represents one of the most promising candidates in catalysis membrane for water decontamination. However, unravelling the intricate relationships between synthesis‐structure–properties remains a great challenge. This study addresses the impacts of coordination environment and structure units of metal central sites based on Mantel test, correlation analysis, and evolution of metal central sites. An optimized unconventional oxygen doping cooperated with Co‐N‐Fe dual‐sites (OCN Co/Fe) exhibits synergistic mechanism for efficient peroxymonosulfate activation, which benefits from a significant increase in charge density at the active sites and the regulation in the natural population of orbitals, leading to selective generation of SO 4 •− . Building upon these findings, the OCN‐Co/Fe/PVDF composite membrane demonstrates a 33 min −1 ciprofloxacin (CIP) rejection efficiency and maintains over 96% CIP removal efficiency (over 24 h) with an average permeance of 130.95 L m −2 h −1 . This work offers a fundamental guide for elucidating the definitive origin of catalytic performance in advance oxidation process to facilitate the rational design of separation catalysis membrane with improved performance and enhanced stability.
The activation of persulfates to degrade refractory organic pollutants is a hot issue in advanced oxidation right now. Here, it is reported that single‐atom Fe‐incorporated carbon nitride (Fe‐CN‐650) can effectively activate peroxymonosulfate (PMS) for sulfamethoxazole (SMX) removal. Through some characterization techniques and DFT calculation, it is proved that Fe single atoms in Fe‐CN‐650 exist mainly in the form of Fe‐N 3 O 1 coordination, and Fe‐N 3 O 1 exhibited better affinity for PMS than the traditional Fe‐N 4 structure. The degradation rate constant of SMX in the Fe‐CN‐650/PMS system reached 0.472 min −1 , and 90.80% of SMX can still be effectively degraded within 10 min after five consecutive recovery cycles. The radical quenching experiment and electrochemical analysis confirm that the pollutants are mainly degraded by two non‐radical pathways through 1 O 2 and Fe(IV)═O induced at the Fe‐N 3 O 1 sites. In addition, the intermediate products of SMX degradation in the Fe‐CN‐650/PMS system show toxicity attenuation or non‐toxicity. This study offers valuable insights into the design of carbon‐based single‐atom catalysts and provides a potential remediation technology for the optimum activation of PMS to disintegrate organic pollutants.
The application of nanotechnology in phytoremediation of heavy-metal-polluted soil has revitalized this traditional remediation technology with higher efficiencies. Among various material types, micronutrient-based nanomaterials have recently come into the public spotlight because of their positive effects on plant performances without significant perturbation to the environmental media, while their effects and the related mechanisms to enhance the phytoremediation efficiencies remain largely uncovered. In this study, molybdenum trioxide nanoparticles (MoO3 NPs) and molybdate (Mo6+) were applied in combined heavy-metal-contaminated soils to explore their effects on plant tolerance and phytoextraction ability of a typical Cd hyperaccumulator, Solanum nigrum L. Experimental results indicated that low-level Mo (4 mg kg–1) application, especially for MoO3 NPs, significantly improved the plant performance and Cd accumulation of S. nigrum by activating nutrient assimilation and antioxidative levels, while excessive Mo addition (20 and 40 mg kg–1) further exacerbated detrimental effects on plants under combined heavy-metal pressure. Furthermore, nontargeted metabolomic analysis was adopted to uncover the regulating mechanisms of Mo materials on plant responses. Under 4 mg kg–1 treatment, MoO3 NPs stimulated metabolite expression related to carbohydrate biosynthesis and antioxidative systems to enhance plant tolerance and phytoextraction ability, revealing less metabolic perturbation compared to Mo6+ treatment. Abscisic acid signaling was considered to be a key regulator contributing to differential regulating pathways between low-level Mo6+ and MoO3 NPs treatments. However, under higher Mo levels, both materials led to similar dysregulations in several important pathways concerning amino acid, lipid, and carbohydrate metabolisms. This study provided a theoretical basis for utilizing essential micronutrient-based nanomaterials to facilitate phytoremediation by hyperaccumulators during in situ remediation of heavy metals.
The development of high-performance catalysts plays a crucial role in facilitating chemical production and reducing environmental contamination. Single-atom catalysts (SACs), a class of catalysts that bridge the gap between homogeneous and heterogeneous catalysis, have garnered increasing attention because of their unique activity, selectivity, and stability in many pivotal reactions. Meanwhile, the scarcity of precious metal SACs calls for the arrival of cost-effective SACs. Cobalt, as a common non-noble metal, possesses tremendous potential in the field of single-atom catalysis. Despite their potential, reviews about single-atom Co catalysts (Co-SACs) are lacking. Accordingly, this review thoroughly summarized various preparation methodologies of Co-SACs, particularly pyrolysis; its application in the specific domain of organic synthesis and environmental remediation is discussed as well. The structure-activity relationship and potential catalytic mechanism of Co-SACs are elucidated through some representative reactions. The imminent challenges and development prospects of Co-SACs are discussed in detail. The findings and insights provided herein can guide further exploration and development in this charming area of catalyst design, leading to the realization of efficient and sustainable catalytic processes.
Emerging evidence from genomics gives us a glimpse into the potential contribution of lysogenic bacteriophages (phages) to the environmental adaptability of their hosts. However, it is challenging to quantify this kind of contribution due to the lack of appropriate genetic markers and the associated controllable environmental factors. Here, based on the unique transformable nature of arsenic (the controllable environmental factor), a series of flooding microcosms was established to investigate the contribution of arsM-bearing lysogenic phages to their hosts' adaptation to trivalent arsenic [As(III)] toxicity, where arsM is the marker gene associated with microbial As(III) detoxification. In the 15-day flooding period, the concentration of As(III) was significantly increased, and this elevated As(III) toxicity visibly inhibited the bacterial population, but the latter quickly adapted to As(III) toxicity. During the flooding period, some lysogenic phages re-infected new hosts after an early burst, while others persistently followed the productive cycle (i.e., lytic cycle). The unique phage-host interplay contributed to the rapid spread of arsM among soil microbiota, enabling the quick recovery of the bacterial community. Moreover, the higher abundance of arsM imparted a greater arsenic methylation capability to soil microbiota. Collectively, this study provides experimental evidence for lysogenic phages assisting their hosts in adapting to an extreme environment, which highlights the ecological perspectives on lysogenic phage-host mutualism.
Catalyst-free visible light assisted Fenton-like catalysis offers opportunities to achieve the sustainable water decontamination, but the synergistic decontamination mechanisms are still unclear, especially the effect of proton transfer process (PTP). The conversion of peroxymonosulfate (PMS) in photosensitive dye-enriched system was detailed. The photo-electron transfer between excited dye and PMS triggered the efficient activation of PMS and enhanced the production of reactive species. Photochemistry behavior analysis and DFT calculations revealed that PTP was the crucial factor to determine the decontamination performance, leading to the transformation of dye molecules. The excitation process inducing activation of whole system was composed of low energy excitations, and the electrons and holes were almost contributed by LUMO and HOMO. This work provided new ideas for the design of catalyst-free sustainable system for efficient decontamination.
Catalyst‐free visible light assisted Fenton‐like catalysis offers opportunities to achieve the sustainable water decontamination, but the synergistic decontamination mechanisms are still unclear, especially the effect of proton transfer process (PTP). The conversion of peroxymonosulfate (PMS) in photosensitive dye‐enriched system was detailed. The photo‐electron transfer between excited dye and PMS triggered the efficient activation of PMS and enhanced the production of reactive species. Photochemistry behavior analysis and DFT calculations revealed that PTP was the crucial factor to determine the decontamination performance, leading to the transformation of dye molecules. The excitation process inducing activation of whole system was composed of low energy excitations, and the electrons and holes were almost contributed by LUMO and HOMO. This work provided new ideas for the design of catalyst‐free sustainable system for efficient decontamination.
The characterization of variations in riverine microbiota that stem from contaminant sources and transport modes is important for understanding biogeochemical processes. However, the association between complex anthropogenic nitrogen pollution and bacteria has not been extensively investigated owing to the difficulties faced while determining the distribution of nitrogen contaminants in watersheds. Here, we employed the Soil and Water Assessment Tool alongside microbiological analysis to explore microbial characteristics and their responses to complex nitrogen pollution patterns. Significant variations in microbial communities were observed in sub-basins with distinct land-water pollution transport modes. Point source-dominated areas (PSDAs) exhibited reduced microbial diversity, high number of denitrification groups, and increased nitrogen cycling compared with others. The negative relative deviations (-3.38) between the measured and simulated nitrate concentrations in PSDAs indicated that nitrate removal was more effective in PSDAs. Pollution sources were also closely associated with microbiota. Effluents from concentrated animal feeding operations were the primary factors relating to the microbiota compositions in PSDAs and balanced areas. In nonpoint source-dominated areas, contaminants from septic tanks become the most relevant sources to microbial community structures. Overall, this study expands our knowledge regarding microbial biogeochemistry in catchments and beyond by linking specific nitrogen pollution scenarios to microorganisms.
Fe/PCN nanomaterial synthesized via a one-step self-assembly strategy was proposed to provide guidance for the removal of OTC.
Conjugated microporous polymers (CMPs) as a new type of conjugated polymers have attracted extensive attention in academia and industry because of the combination of microporous structure and π-electron conjugated structure. The construction and application of gels and monoliths based on CMPs constitute a fertile area of research, promising to provide solutions to complex environmental and energy issues. This review summarizes and objectively analyzes the latest advances in the construction and application of processable CMP gels and monoliths, linking the basic and enhanced properties to widespread applications. In this review, we open with a summary of the construction methods used to build CMP gels and monoliths and assess the feasibility of different preparation techniques and the advantages of the products. The CMP gels and monoliths with enhanced properties involving various special applications are then deliberated by highlighting relevant scientific literature and discussions. Finally, we present the issues and future of openness in the field, as well as come up with the major challenges hindering further development, to guide researchers in this field.
Simultaneous regulation of the coordination environment of single‐atom catalysts (SACs) and engineering architectures with efficient exposed active sites are efficient strategies for boosting peroxymonosulfate (PMS) activation. We isolated cobalt atoms with dual nitrogen and oxygen coordination (Co−N 3 O 1 ) on oxygen‐doped tubular carbon nitride (TCN) by pyrolyzing a hydrogen‐bonded cyanuric acid melamine–cobalt acetate precursor. The theoretically constructed Co−N 3 O 1 moiety on TCN exhibited an impressive mass activity of 7.61×10 5 min −1 mol −1 with high 1 O 2 selectivity. Theoretical calculations revealed that the cobalt single atoms occupied a dual nitrogen and oxygen coordination environment, and that PMS adsorption was promoted and energy barriers reduced for the key *O intermediate that produced 1 O 2 . The catalysts were attached to a widely used poly(vinylidene fluoride) microfiltration membrane to deliver an antibiotic wastewater treatment system with 97.5 % ciprofloxacin rejection over 10 hours, thereby revealing the suitability of the membrane for industrial applications.
Simultaneous regulation of the coordination environment of single‐atom catalysts (SACs) and engineering architectures with efficient exposed active sites are efficient strategies for boosting peroxymonosulfate (PMS) activation. We isolated cobalt atoms with dual nitrogen and oxygen coordination (Co−N 3 O 1 ) on oxygen‐doped tubular carbon nitride (TCN) by pyrolyzing a hydrogen‐bonded cyanuric acid melamine–cobalt acetate precursor. The theoretically constructed Co−N 3 O 1 moiety on TCN exhibited an impressive mass activity of 7.61×10 5 min −1 mol −1 with high 1 O 2 selectivity. Theoretical calculations revealed that the cobalt single atoms occupied a dual nitrogen and oxygen coordination environment, and that PMS adsorption was promoted and energy barriers reduced for the key *O intermediate that produced 1 O 2 . The catalysts were attached to a widely used poly(vinylidene fluoride) microfiltration membrane to deliver an antibiotic wastewater treatment system with 97.5 % ciprofloxacin rejection over 10 hours, thereby revealing the suitability of the membrane for industrial applications.
Modulating the structure of Fe catalysts is possible to alter the exposure of active sites, electron density around active sites, coordination number, charge transfer or mass transfer limitation, and thus affect Fenton-like catalytic activity.
Versatile types of MOF-derived mixed transition metal nanomaterials are summarized in terms of synthetic routes. The applications of those materials in energy storage and conversion, including LIBs, SCs, ORR, OER and HER are discussed.
The addition of nZVI could improve the degradation efficiency for chlorophenothane using chicken manure compost, while the compost mitigated the negative effect of nZVI on the bacterial community structure in sediment.
Nowadays, to alleviate the growing pressure of energy shortages and environmental pollution, electrochemical energy conversion is seen as a fossil‐free, secondary pollution‐free, and highly efficiency pathway. Electrocatalysts, as the “heart” of the electrochemical conversion process, play a key role in accelerating reaction rates and promoting efficiency. Transition‐metal‐based layered double hydroxides (TM LDHs), one of the famous electrocatalysts, show unique 2D supermolecular‐stratified structure, excellent electronic properties, and their raw materials are easily available. In this review, electrocatalysis‐related properties of TM LDHs and the state‐of‐the‐art synthesis methods of TM LDH‐based electrocatalysts are summarized. Modifications for promoting the development of TM LDH‐based electrocatalysts are included, such as carbon materials modification, defect engineering, and noble metal loading. Then, the application of TM LDH nanosheets in the field of electrocatalysis is reviewed in detail. Finally, recent challenges, ongoing improvements, and future expectations for TM LDH nanosheets are presented.
Strategies to improve the photocatalytic activity of PDI are summarized. The system factor and water chemistry affecting the photocatalytic activity for organic pollutant removal are discussed. The stability and future challenges are discussed.