Latest ArticlesWastewater management and energy/resource recycling have been extensively investigated via photo(electro)catalysis. Although both operation processes are driven effectively by the same interfacial charge, each system is practiced separately since they require very different reaction conditions. In this review, we showcase the recent advancements in photo(electro)catalytic process that enables the wastewater treatment and simultaneous energy/resource recovery (WT-ERR). Various literatures based on photo(electro)catalysis for wastewater treatment coupled with CO2 conversion, H2 production and heavy metal recovery are summarized. Besides, the fundamentals of photo(electro)catalysis and the influencing factors in such synergistic process are also presented. The essential feature of the catalysis lies in effectively utilizing hole oxidation for pollutant degradation and electron reduction for energy/resource recovery. Although in its infancy, the reviewed technology provides new avenue for developing next-generation wastewater treatment process. Moreover, we expect that this review can stimulate intensive researches to rationally design photo(electro)catalytic systems for environmental remediation accompanied with energy and resource recovery.
Available online An efficient method for the synthesis of multi-substituted cyclic imides was developed with cyanoesters and diaryliodonium salts. This method proceeds through a cascade of N-arylation-acylation and rearrangement to give target heterocycles in good yields (up to 99%). This method has the major advantages of a broad substrate scope, excellent functional group compatibility. The strategy was also extended to the fused cyclic imides, such as malonimides, succinimides and glutarimides.
The oxygen reduction reaction (ORR), an important process in Zn-air batteries (ZABs), shows sluggish reaction kinetics, which significantly impairs the further improvement of battery performance. Thus, rationally designing cathodic catalysts for ZABs has drawn sufficient attention. We herein synthesize and characterize Fe/N/F-tridoped CNTs (FeNFCs) by annealing the postsynthesized trifluoroacetic anhydride-modified Fe-MIL-88B-NH2 nanocrystals with melamine at high temperature in a N2 atmosphere. Benefiting from the Fe/N/F element doping, high specific surface area, and CNT structure, the FeNFC800 catalyst prepared at 800 ℃ exhibits a preferable half-wave potential of 0.829 V vs. RHE. The Zn-air battery equipped with FeNFC800 shows a high open-circuit voltage of 1.47 V, a gratifying peak power density of 196 mW/cm2, and extraordinary long-term stability, outperforming the benchmark 20% Pt/C.
High residual concentration of arsenic and fluoride is a tricky problem to be solved in the process of reinjection after geothermal water utilization. We develop a method to simultaneously remove As(Ⅴ) and F− from geothermal water using magnetic Fe3O4@MgO adsorbent, fabricated via a one-step method. The effects of pH, contact time, adsorbent dose and temperature on the removal efficiency were investigated systematically. The results show that the Fe3O4@MgO composite has a wide range of pH (2–11), ultrafast removal dynamics (As(Ⅴ): 2 min; F−: 30 min), and high removal efficiency (As(Ⅴ): 99.9%; F−: 96.6%). The adsorption kinetics follows the pseudo-second-order kinetics model, and the adsorption isotherm model fits Freundlich. The adsorption capacity of As(Ⅴ) and F− can reach 123 and 98.4 mg/g, respectively. The exchange of As(Ⅴ) and F− with Mg-hydroxyl groups hydrolysis by MgO was determined the adsorption mechanism. The Fe3O4@MgO adsorbent was capable of achieving the adsorption efficiency as high as 99.9% for As(Ⅴ) and 97.3% for F− in real geothermal water, respectively. Hence, the proposed Fe3O4@MgO composite exhibited as an excellent adsorbent for the remediation of As- and F-contaminated geothermal water.
Understanding the influence of sulfates over catalysts for selective catalytic reduction of NO with NH3 (NH3-SCR) is crucial due to the universal presence of SO2 in exhaust gas. Depending on the degree of sulfation, there mainly exist surface and bulk sulfates and NH3-SCR activity is generally considered to suffer more from bulk sulfates. Herein, the unique function of bulk sulfates over CeO2 in promoting high-temperature SCR reaction is revealed. Notably, compared with CeO2 dominated with surface sulfates (S-CeO2–4h) and commercial V2O5-WO3/TiO2, CeO2 with bulk sulfates (S-CeO2–72h) exhibits admirable NO conversion at the temperature range of 400–550 ℃. Bulk sulfates provide more Brønsted acid sites with stronger strength for NH3 adsorption. Moreover, the oxidation ability of CeO2 is significantly inhibited due to electron-withdrawing effect from bulk sulfates, which alleviates NH3 oxidation at high temperatures. More NH3 adsorption with high stability and limited NH3 oxidation capacity ensure the excellent catalytic performance for S-CeO2–72h in high-temperature denitration. This work provides new insight of bulk sulfates in promoting SCR activity and open a new avenue to design deNOx catalysts employed at high temperatures.
Novel polyoxometalate (POM) Pickering interfacial catalyst (PIC) was fabricated through loading (NH4)5H6PMo4V8O40 (PMo4V8) on both alkyl and alkyl-amino groups functionalized silica nanoparticles. PMo4V8/SiO2(C8/C8NH2 with molar ratio as 1:1) PIC system provided a new catalytic model for aerobic conversion of 5-hydroxymethylfurfural (5-HMF), as well as its recovery and product separation in H2O/methyl isobutyl ketone (MIBK) biphase reaction. Balancing the ratio of PMo4V8, C8 and C8NH2 gave rise to variety in hydrophilicity and hydrophobicity for PMo4V8/SiO2(C8/C8NH2), which enhanced the transformation of 5-HMF to 2, 5-diformylfuran (DFF) in H2O/MIBK with 73.7% yield at 81.8% conversion than in H2O or MIBK single phase.
Tyrosine sulfation is an important post-translational modification that enhances the inhibitory activity of hirudin. Herein, we developed a facile synthetic strategy to afford the sulfated hirudins with up to three modifications and in multi-milligram scales, after a single HPLC purification step. Through these synthetic proteins, a novel type of modulation mechanism exhibited by tyrosine sulfation was proposed, which would help to delineate the structure–function relationships in other sulfated proteins and more importantly, to serve as a basis for the development of related antithrombotic agents.
Comprehensive surgical staging or optimal tumor cytoreductive surgery of malignant ovarian cancer directly affects disease prognosis. Therefore, a fluorescent selenium nanoparticle (Se@RGD/S2.2) decorated with cancer-targeting Arg-Gly-Asp (RGD) peptides and GCAGTTGATCCTTTGGATACCCTGG aptamer (S2.2) was developed for use as a diagnostic agent to achieve rapid, noninvasive diagnosis and visualization of microinvasive lesions during surgery for malignant ovarian cancer.
Two erbium(Ⅲ) complexes [ErCl(OArAd)3][Na(THF)6] (1) and Er(OArAd)3 (2) are successfully prepared by using one variety of "hard" base ligand with large steric hindrance. The coordination geometry around the Er(Ⅲ) site changes from distorted tetrahedral to flat trigonal pyramid geometry in different solvent environment due to the removal of the coordinated chloride. Such an alternation significantly enhances the single-molecule magnet (SMM) behavior and makes the field-induced effective energy barrier (Ueff) arrive at 43(1) cm−1 for the latter. Together with theoretical calculations, this study shows that strong equatorial ligand field and high local symmetry are critical to suppress the quantum tunneling of the magnetization (QTM) and achieve high-performance erbium(Ⅲ) based SMMs.
More and more antibiotics that are difficult to biodegrade have been detected in water environments threatening ecosystems and human health. Therefore, it is urgent to develop efficient water treatment methods to degrade antibiotics. In this work, Co-Fe Prussian blue analogues (PBAs) with different molar ratios were synthesized for peroxymonosulfate (PMS) activation to degrade sulfacetamide (SAM, 10 mg/L). By increasing Co molar ratio, the PMS activation capability and electrochemical properties of PBAs were enhanced. Due to its excellent reactivity (degradation efficiency of 84.2% and mineralization efficiency of 52.79%), cost benefit (electrical energy per order, 0.01019 kWh/L) and lower metal leaching ([Co] = 0.259 mg/L, [Fe] = 0.128 mg/L), PBA-1, the as-prepared catalyst with a molar ratio of cobalt to iron of 1:1, was selected for further study. The radical scavenging experiments and an electron paramagnetic resonance (EPR) trapping experiments were performed and revealed that PBA-1 addition was required to produced •OH and SO4•− from PMS activation. Accordingly, we proposed a PMS activation mechanism and SAM decomposition pathways for PBA-1/PMS reaction system. Besides, a PBA-1@polyvinylidene fluoride (PVDF) catalytic membrane was further prepared to expand the application potential of PBA nanoparticles. The PBA-1@PVDF catalytic membrane was highly effective and exhibited a great reusability; thus, it could be considered for applications in actual water treatment processes.
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