A Regenerable Cu2O/BiOBr S-scheme Heterojunction Photocatalysts for Efficient Photocatalytic Degradation of Mixed Organic Pollutants

Oxygen vacancies-rich Cu-W18O49 nanorods supported on reduced graphene oxide for electrochemical reduction ofN2to NH3.

Improving the activation capacity of peroxymonosulfate (PMS) to increase radical and non-radical production is critical for antibiotic degradation. However, how to boost reactive oxygen species (ROS) and speed interfacial charge transfer remains an essential challenge. We report a coupling system of 10 %CNNS/CuBi2O4 photocatalyst and sulfate radical-based advanced oxidation processes (SO4−-AOPs) to enhance the activation of PMS and improve antibiotic degradation. Owing to highly efficient oxygen activation and interfacial charge transfer, the degradation efficiency of the photo-assisted PMS system was as high as 51.6 times and 2.8 times that of photocatalyst and SO4−-AOPs alone, respectively. Importantly, the highly efficient oxygen activation resulted in the production of O2−, which in turn could utilize the excess electrons generated through efficient interfacial charge transfer to convert into non-radical 1O2. The total organic carbon (TOC) elimination effectiveness of the photo-assisted PMS system reached 82 % via the synergy of radicals and non-radicals (O2−, OH, 1O2, SO4−, h+). This system also had excellent potential for reducing the generation and toxicity of disinfection by-products (DBPs), as evidenced through significant reductions in concentrations of trichloromethane (TCM), dichloroacetic acid (DCAA), and trichloronitromethane (TCNM) by 76 %, 64 %, and 35 %, respectively, providing an effective and eco-friendly strategy for antibiotic treatment. 

Enhanced antibiotic degradation via photo-assisted peroxymonosulfate over graphitic carbon nitride nanosheets/CuBi2O4: Highly efficiency of oxygen activation and interfacial charge transfer

Reasonably designing and constructing efficient artificial S-mechanism photocatalysts, expanding their application in the field of photocatalytic organic synthesis, have become a hot and challenging topic in the photocatalysis. Herein, a series of coral-like W18O49@TpPa-H (TpPa-H represents COFs generated by the reaction of 1,3,5-triformylphloroglucinol (Tp) and p-phenylenediamine (Pa-H)) composites were successfully prepared by using a simple in-situ encapsulation strategy. Given the internal electric field at the S-scheme interface, W18O49 acts as an oxidative photocatalyst with sufficient positive valence band (VB) position and TpPa-H as a reductive one with enough negative conduction band (CB) position for the efficient amines oxidative coupling to imines. The resulting W18O49@TpPa-H-0.1 hybrid material shows both optimal benzylamine to imine conversion and selectivity exceeding 99 % within 4 h under 10 W 420 nm LED light irradiation, which is 9.9 and 2.8 fold greater than that of W18O49 and TpPa-H, respectively. The photocatalytic activity is even extended to 740 nm. Furthermore, the photocatalytic mechanism research confirmed that a high efficiency S-scheme heterojunction was formed between W18O49 and TpPa-H, and multiple active species, such as ·O2–, 1O2, and h+, synergistically participated in the reaction, imparting its excellent photocatalytic performance. This work may open new avenues for the development of high-efficiency COFs-based S-scheme heterojunction for organic photosynthesis. 

Coralloid W18O49@Covalent Organic Frameworks S-scheme Heterojunction for High Efficiency Photocatalytic Aerobic Oxidation

Electrocatalytic nitrogen reduction (NRR) for artificial ammonia synthesis under ambient conditions is considered a promising alternative to the traditional Haber-Bosch process. However, it still faces multiple challenges such as the...

A simple hydrothermal synthesis of oxygen vacancy-rich MnMoO4 rod-like materials and its highly efficient electrocatalytic nitrogen reduction

The Enhanced Photocatalytic Performance of the Amorphous Carbon/Mgo Nanofibers: Insight into the Role of the Oxygen Vacancies and 1d Morphology

Efficient carriers separation and multiple nitrogen (N2) activation sites are essential for N2 photo-fixation. Here, we found that the BiOBr/TiO2 (BBTO) displayed an attractive reversible photochromism (white → grey) due to the generation of electron deficient Bi3+δ, which was produced by the hole trapping of Bi3+ under light irradiation. Interestingly, more Bi3+δ were detected in the BBTO heterojunction than in pure BiOBr, attributing that the hole trapping was promoted by the built-in electric field in the Step scheme (S-scheme) heterojunction. In the BBTO, the electron deficient Bi3+δ enhanced carriers separation and served as the reactive active site to adsorb more N2. Consequently, the BBTO possessed an excellent N2 photo-fixation activity (191 μmol gcat-1 h-1), which was 7.7 and 18 times higher than that of pure BiOBr (24.8 μmol gcat-1 h-1) and TiO2 (10.6 μmol gcat-1 h-1), respectively. Therefore, this work provides a new perspective for enhancing N2 photo-fixation by the electron deficient photocatalysts with S-scheme heterojunction. 

Electron deficient Bi3+δ serves as N2 absorption sites and inhibits carriers recombination to enhance N2 photo-fixation in BiOBr/TiO2 S-scheme heterojunction.

NH3 is considered as an ideal fuel for fuel cells to achieve zero carbon emissions due to its high energy density (at liquefaction) and carbon-free properties. The zero-carbon clean electrocatalytic nitrogen reduction reaction (NRR) is one of the alternative routes for NH3 synthesis. The efficiency of NRR is restricted by the high stability of N N and the slow reaction rate. In this study, La2(MoO4)3 (LaMo), and x%Fe doping-LaMo (x = 3, 5, 7, and 10) are synthesized via a hydrothermal method. The strong electron-donating ability of Fe converts a part of Mo6+ to Mo5+ and Mo4+ improving the electronic environment. The presence of Mo5+, an intermediate valence state, facilitates the oxidation and reduction reactions and establishes rapid electron transport channels. The electron transport of Mo6+↔e−Mo5+ is easier than Mo6+↔2e−Mo4+. Furthermore, the Mo5+ activates N2 and enhances N2 adsorption, boosting the NRR performance. Importantly, the content of Mo5+ exhibits a positive correlation with NH3 yield rate (R2 = 0.89), and Faradaic efficiency (FE, R2 = 0.95). Consequently, the 5%Fe–LaMo exhibits the highest Mo5+ percentage (75.9 %) and NRR performance (NH3 yield rate:30.4 μg h−1 mgcat−1, FE: 3.6 %). Thus, this study proposes a method to enhance the NRR performance by element doping with strong electron-donating ability to regulate the Mo5+ percentage. 

The intermediate valence state Mo5+ in Fe doping La2(MoO4)3 boosting electrochemical nitrogen reduction

The achievement of the outstanding theoretical capacitance of nickel sulfide (NiS2) is challenging due to its low conductivity, slow electrochemical kinetics, and poor structural stability. In this study, we utilize polyaniline (PANI) as a linker to anchor the NiS2 with a hollow bowl-like structure, uniformly dispersed at the surface of graphene oxide (GO)(NiS2@15PG). The presence of PANI provides growth sites, resulting in a uniform and dense arrangement of NiS2. This morphological modulation of NiS2 increases the contact area between the active material to electrolyte. Additionally, PANI effectively connects NiS2 with the conductive network of GO, which advances the electrical conductivity and ion diffusion properties. As a result, the Rct (charge transfer resistance) and Zw (Warburg impedance) of NiS2@15PG decrease by 82.61% and 66.76% respectively. This unique structure confers NiS2@15PG with high specific capacitance (536.13 C g-1 at 1 A g-1) and excellent multiplicative property of 60.93% at 20 A g-1. The assembled NiS2@15PG//YP-50 supercapacitors (HSC) demonstrate an energy density (13.09 Wh kg-1) at a high-power density (16000 W kg-1). The capacity retention after 10,000 cycles at 5 A g-1 is 86.59%, indicating its significant potential for practical applications.

Hollow bowl NiS2@polyaniline conductive linker/graphene conductive network: a triple composite for high-performance supercapacitor applications.

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