Search

Conventional advanced oxidation processes (AOPs) require significant external energy consumption to eliminate emerging contaminants (ECs) with stable structures. Herein, a catalyst consisting of nanocube BiCeO particles (BCO‐NCs) prepared by an impregnation‐hydrothermal process is reported for the first time, which is used for removing ECs without light/electricity or any other external energy input in water and simultaneous in situ generation of H2O2. A series of characterizations and experiments reveal that dual reaction centers (DRC) which are similar to the valence band/conducting band structure are formed on the surface of BCO‐NCs. Under natural conditions without any external energy consumption, the BCO‐NCs self‐purification system can remove more than 80% of ECs within 30 min, and complete removal of ECs within 30 min in the presence of abundant electron acceptors, the corresponding second‐order kinetic constant is increased to 3.62 times. It is found that O2 can capture electrons from ECs through the Bi─O─Ce bond bridge during the reaction process, leading to the in situ production of H2O2. This work will be a key advance in reducing energy consumption for deep wastewater treatment and generating important chemical raw materials. [ABSTRACT FROM AUTHOR]

Graphical abstract Highlights • Mo S C and Mo O Co electron transfer bridges are successfully constructed on CMS-rGO NSs. • CMS-rGO NSs possesses the function of generating and activating H 2 O 2 synchronously. • CMS-rGO NSs shows very high Fenton-like activity for degradation of pollutants. • Dye pollutants can directly act as electron donors for CMS-rGO NSs. Abstract Consumption of additional H 2 O 2 is necessary in classical Fenton catalysis. Herein, we report a novel and special nanocatalyst consisting of CoMoS 2 nanosphere-embedded, reduced graphene oxide (rGO) nanosheets (CMS-rGO NSs). This nanocatalyst was discovered to have an impressive reactivity for in situ generation and synchronistical activation of H 2 O 2 in different active centers, yielding fast and efficient degradation of the pollutants. The reaction rate is ∼21 times higher than that of conventional Fenton catalysts. The characterization shows that countless flower-like CoMoS 2 nanospheres are uniformly embedded in the rGO nanosheets through Mo S C bonding bridges in CMS-rGO NSs, which leads to activation of the π electrons and their transfer from rGO to the metal centers (π → M). The formed Mo O Co further leads to a distribution of orientations of the electrons around the metal centers due to the different electronegativity of Mo and Co. During the reaction, the dissolved O 2 is efficiently reduced to HO 2 /O 2 − around the electron-rich Mo center, and HO 2 /O 2 − is further reduced to H 2 O 2 around the Co center. The generated H 2 O 2 is finally reduced to OH for degrading dyes in the electron-rich metal (Mo or Co) centers of CMS-rGO NSs. The dye pollutants also act as electron donors, and they are directly degraded in the electron-poor π-center of CMS-rGO NSs, which promote the electron transfer cycle and achieve electron gain-loss balance. This discovery provides a new strategy for H 2 O 2 generation-activation and pollutant degradation through constructing electron transfer bridges over the surface of catalysts. [ABSTRACT FROM AUTHOR]

[Display omitted] • Surface microelectric fields (SMEF) on catalyst were formed by electrostatic force. • The formation of SMEF maximize the removal of refractory pollutants in wastewater. • The SMEF can link electron transfer between refractory pollutants and microorganisms. • The interspecific electron transport was induced by SMEF to can speed up degradation. The stable structure and toxic effect of refractory organic pollutants in wastewater lead to the problem of high energy consumption in water treatment technology. Herein, we propose a synergistic purification of refractory wastewater driven by microorganisms and surface microelectric fields (SMEF) over a dual-reaction-center (DRC) catalyst HCLL-S8-M prepared by an in situ growth method of carbon nitride on the Cu-Al 2 O 3 surface. Characterization techniques demonstrate the successful construction of SMEF with strong electrostatic force over HCLL-S8-M based on cation-π interactions between metal copper ions and carbon nitride rings. With the catalyst as the core filler, an innovative fixed bed bioreactor is constructed to purify the actual kitchen-oil wastewater. The removal efficiency of the wastewater even with a very low biodegradability (BOD 5 /COD = 0.33) can reach 60% after passing through this bioreactor. An innovative reaction mechanism is revealed for the first time that under the condition of a small amount of biodegradable organic matter, the SMEF induces the enrichment of electric active microorganisms (Desulfobulbus and Geobacter) in the wastewater, accelerates the interspecies electron transfer of intertrophic metabolism with the biodegradable bacteria through the extracellular electron transfer mechanism such as cytochrome C and self-secreted electron shuttle. The electrons of the refractory organic pollutants adsorbed on the surface of the catalyst are delocalized by the SMEF, which can be directly utilized by microorganisms through EPS conduction. The SMEF generated by electron polarization can maximize the utilization of pollutants and microorganisms in wastewater and further enhance degradation without adding any external energy, which is of great significance to the development of water self-purification technology. [ABSTRACT FROM AUTHOR]

• Co2+-N-C π is constructed via atomically dispersed Co bonding with C-based graphene-like structure. • Co2+-N-C π (Co−π) structure plays key role for PMS activation and pollutant degradation. • Electron donation effect of pollutants is realized through π-π interaction in SACo-NGs system. • High efficiency and low consumption are realized in SACo-NGs/PMS water treatment system. Orbital interaction involving metal cation−π is an important form for electron transfer regulation. To accelerate the interfacial electron transfer of peroxymonosulfate (PMS) activation for water treatment, we report a new strategy through bonding atomically dispersed cobalt with nanospheric C-based graphene-like structures (SACo-NGs) to form metal cation−π structure, driving rapid and directional transfer of the electrons of pollutants to PMS on the catalyst surface. The catalyst SACo-NGs is synthesized by an enhanced hydrothermal-sintering method and the formation of metal cation−π structure is demonstrated by X-ray absorption fine structure (EXAFS), X-ray photoelectron spectroscopy (XPS), electron paramagnetic resonance spectroscopy (EPR) and Raman spectroscopy. It is found that Co−π structures (Co2+-N-C π) play a key role for the efficient activation of PMS, which results in pollutants being greatly removed in a few minutes. During the reaction, pollutants can donate electrons for the system through π−π interaction accompanying by the direct oxidative degradation of pollutants. The obtained electrons are quickly transferred to the atomically dispersed cobalt sites through the formed cation−π structure, which promotes the activation of PMS. This is a successful practice in the field of PMS activation using cation−π structure to accelerate electron transfer and achieve rapid degradation of pollutants. [ABSTRACT FROM AUTHOR]

The effects of biological activated carbon treatment using Fe 2 O 3 modified coconut shell-based activated carbon (Fe/CAC) were investigated on the occurrence of opportunistic pathogens (OPs) and formation of disinfection by-products (DBPs) in simulated drinking water distribution systems (DWDSs) with unmodified CAC as a reference. In the effluent of annular reactor (AR) with Fe/CAC, the OPs growth and DBPs formation were inhibited greatly. Based on the differential pulse voltammetry and dehydrogenase activity tests, it was verified that extracellular electron transfer was enhanced in the attached biofilms of Fe/CAC, hence improving the microbial metabolic activity and biological removal of organic matter especially DBPs precursors. Meanwhile, the extracellular polymeric substances (EPS) on the surface of Fe/CAC exhibited stronger viscosity, higher flocculating efficiency and better mechanical stability, avoiding bacteria or small-scale biofilms falling off into the water. Consequently, the microbial biomass and EPS substances amount decreased markedly in the effluent of Fe/CAC filter. More importantly, Fe/CAC did significantly enhance the shaping role on microbial community of downstream DWDSs, continuously excluding OPs advantage and inhibiting EPS production. The weakening of EPS in DWDSs resulted in decrease of microbial chlorine-resistance ability and EPS-derived DBPs precursors supply. Therefore, the deterioration of water quality in DWDSs was inhibited greatly, sustainably maintaining the safety of tap water. Our findings indicated that optimizing biological activated carbon treatment by interface modification is a promising method for improving water quality in DWDSs. Image 1 • The performance of Fe 2 O 3 /coconut-shell activated carbon (Fe/CAC) was studied. • Fe/CAC enhanced extracellular electron transfer and biodegradation effect. • Less microbes and smaller microbial clusters occurred in the effluent of Fe/CAC. • Fe/CAC enhanced the shaping role on the microbial community of DWDSs. • Fe/CAC further enhanced the water quality in drinking water distribution systems. Fe/CAC did control the microbial biomass, EPS characteristics and microbial community in the water simultaneously, maintaining the safety of tap water. [ABSTRACT FROM AUTHOR]

[Display omitted] • Pigeon manure biochar with electron poor/rich regions on the surface. • Biochar (5 g/L) can significantly increase cumulative methane production. • Adding biochar facilitated the enrichment of methanogenic archaea. • Metagenomes reveal synergistic mechanisms between functional microbes. Inefficient electron transfer is a key bottleneck for anaerobic digestion (AD), which often leads to system instability. Here, we propose for the first time a new strategy to solve the problem by adding surface electron-polarized biochar to enhance methanogenesis by providing electrons to methanogens through surface electron-poor/rich regions. Pyrolysis conversion of pigeon manure to conductive materials (CM) containing electron-poor/rich regions is realized. Different levels of CM (2.5, 5 and 7.5 g/L) are used to enhance methane production from pig manure and rice straw co-digestion systems. It is found that the addition of 5 g/L CM results in the highest cumulative CH 4 production (187.4 ± 8.0 mL/g VS substrate), 35.4% higher (P < 0.05) than the control (0 g/L). Methanogenic archaea are enriched. Synergistic metabolic mechanisms between the functional microorganism bin.CM52.160 (cellulose degradation) and bin.CM03.101 (methane production) are revealed by the metagenomic binning strategy. A large number of potentially unculturable electroactive microorganisms have been identified. This work provides important insights into the construction of micro-electric fields on material surfaces and offers a practical approach to improving AD performance. [ABSTRACT FROM AUTHOR]

In common advanced oxidation processes, excess reagents and energy are often added to the reaction system to maintain the continuity of the reaction. These additions result in a large waste of resources and energy, which has become a bottleneck in the development of water treatment technology. In this study, we propose a new strategy to solve this problem based on a novel dual-reaction-center (DRC) Fe-ZnS quantum dots (Fe–ZnS QDs) catalyst that forms a non-equilibrium surface with an electron-polarized distribution. Through experimental and theoretical studies, it was verified that the activation of trace amounts of H 2 O 2 could break the energy barrier for pollutants to transfer electrons. The dissolved oxygen (DO) in the reaction system could be activated by gaining energy on the surface of the Fe–ZnS QDs catalyst, and was converted to 1O 2 to attack organic pollution. In addition, the pollutants themselves supplied electrons to H 2 O 2 through the surface of the Fe–ZnS QDs catalyst to generate more •OH radicals for pollutant degradation, thus providing two fast paths for pollutant degradation. The system could drive the reaction through a trace amount of H 2 O 2 , thereby activating DO to generate 1O 2 while effectively using the energy of pollutants. Therefore, the proposed system offers a new direction for the development of environmentally-friendly catalysts and greatly reduces the consumption of resources and energy. [Display omitted] • Fe–ZnS QDs is successfully developed as a Fenton catalyst for the first time. • The surface of ZnS QDs is regulated by trace Fe to form a non-equilibrium surface with an electron-polarized distribution. • The Fe–ZnS QDs/H 2 O 2 system exhibits excellent activity for pollutants degradation. • Inert oxygen species in reaction system are easily activated to 1O 2 to attack pollutants. [ABSTRACT FROM AUTHOR]