Atomically Dispersed FeN2 P2 Motif with High Activity and Stability for Oxygen Reduction Reaction Over the Entire pH Range.

The past decade has witnessed the great potential of Fe-based single-atom electrocatalysis in catalyzing oxygen reduction reaction (ORR). However, it remains a grand challenge to substantially improve their intrinsic activity and long-term stability in acidic electrolytes. Herein, we report a facile chemical vapor deposition strategy, by which high-density Fe atoms (3.97 wt%) are coordinated with square-planar para-positioned nitrogen and phosphorus atoms in a hierarchical carbon framework. The as-crafted atomically dispersed Fe catalyst (denoted Fe-SA/PNC) manifests an outstanding activity towards ORR over the entire pH range. Specifically, the half-wave potential of 0.92 V, 0.83 V, and 0.86 V vs. reversible hydrogen electrode (RHE) are attained in alkaline, neutral, and acidic electrolytes, respectively, representing the high performance among reported catalysts to date. Furthermore, after 30,000 durability cycles, the Fe-SA/PNC remains to be stable with no visible performance decay when tested in 0.1 M KOH and 0.5 M H2 SO4 , and only a minor negative shift of 40 mV detected in 0.1 M HClO4 , significantly outperforming commercial Pt/C counterpart. The coordination motif of Fe-SA/PNC is validated by density functional theory (DFT) calculations. This work provides atomic-level insight into improving the activity and stability of non-noble metal ORR catalysts, opening up an avenue to craft the desired single-atom electrocatalysts.

Simultaneous sulfamethoxazole degradation with electricity generation by microbial fuel cells using Ni-MOF-74 as cathode catalysts and quantification of antibiotic resistance genes.

Antibiotic wastewater presents serious challenges in water treatment. Metal-organic frameworks (MOFs) have received significant attention as promising precursors and sacrificial templates in the preparation of porous carbon-supported catalysts. Herein, we investigated the sulfamethoxazole (SMX) degradation and electrochemical performance of microbial fuel cells (MFCs) that applied as-prepared Ni-MOF-74 and Ni-N-C (Ni-MOF-74 underwent pyrolysis treatment at different temperatures) as air-cathode catalyst. Firstly, the electrocatalytic activity towards oxygen reduction reaction (ORR) of the catalyst was investigated by rotating disk electrode. The results showed that electron transfer number for Ni-MOF-74 was 2.12, while that of 800Ni-N-C was 3.44, which was close to four-electron reduction. Applying Ni-MOF-74 in MFCs, a maximum power density of 446 mW/m2 was obtained, which was close to that of 800Ni-N-C. Besides, using Ni-MOF-74 as cathode catalyst, a chemical oxygen demand removal rate of about 84% was obtained, and the degradation rate of 10 mg/L SMX was 61%. The degradation rate decreased with increasing antibiotic concentration, but the average degradation efficiency increased stepwise. Additionally, the relative abundance of resistant gene sul1 in the reactors of the new catalytic material was about 62% lower than that of sul1 in the control (Pt/C) reactors, and the relative abundance of sul2 was about 73% lower. Moreover, cost assessments related to the catalyst performance are presented. The findings of this study demonstrated that Ni-MOF-74 could be considered as a two-electron transfer ORR catalyst, and offers a promising technique for preparation of Ni-N-C for use as four-electron transfer ORR catalysts. In comparison, Ni-MOF-74 could be a promising ORR catalyst of MFCs for antibiotic degradation.

A Bi-Co Corridor Construction Effectively Improving the Selectivity of Electrocatalytic Nitrate Reduction toward Ammonia by Nearly 100.

Improving the selective ammonia production capacity of electrocatalytic nitrate reduction reaction (NO3 RR) at ambient conditions is critical to the future development and industrial application of electrosynthesis of ammonia. However, the reaction involves multi-proton and electron transfer as well as the desorption and underutilization of intermediates, posing a challenge to the selectivity of NO3 RR. Here the electrodeposition site of Co is modulated by depositing Bi at the bottom of the catalyst, thus obtaining the Co+Bi@Cu NW catalyst with a Bi-Co corridor structure. In 50 mm NO3 - , Co+Bi@Cu NW exhibits a highest Faraday efficiency of ≈100% (99.51%), an ammonia yield rate of 1858.2 µg h-1  cm-2 and high repeatability at -0.6 V versus the reversible hydrogen electrode. Moreover, the change of NO2 - concentration on the catalyst surface observed by in situ reflection absorption imaging and the intermediates of the NO3 RR process detected by electrochemical in situ Raman spectroscopy together verify the NO2 - trapping effect of the Bi-Co corridor structure. It is believed that the measure of modulating the deposition site of Co by loading Bi element is an easy-to-implement general method for improving the selectivity of NH3 production as well as the corresponding scientific research and applications.

Degradation pathways, microbial community and electricity properties analysis of antibiotic sulfamethoxazole by bio-electro-Fenton system.

Sulfamethoxazole (SMX) is a general antibiotic that is frequently identified in wastewater and surface water. In this study, the degradation and metabolic pathway of SMX by bio-electro-Fenton systems equipped with a CNT/r-FeOOH cathode were investigated. When initial SMX = 25 mg/L, the removal efficiency of SMX reached 94.66% by the bio-electro-Fenton system. The concentrations of sul1, sul2, sul3, sulA, intI1 and 16S rRNA genes were examined in effluents. Four out of the six ARGs analysed were detected. Among all quantified sul genes, sul1 and sulA were the most abundant. High-throughput sequencing revealed that the microbial communities and relative abundance at the phylum and genus levels were affected by different SMX concentrations. In addition, the intermediates were detected and the possible SMX degradation pathway by the bio-electro-Fenton process in the present system was proposed. Furthermore, the highest power density obtained was 283.32 ± 16.35 mW/m2 (SMX = 25 mg/L). This study provides an efficient and cost effective method for degrading antibiotics.