Metal-organic frameworks (MOFs) have attracted tremendous interest in the photocatalytic hydrogen evolution reaction (HER). Nevertheless, their practical catalytic performance is limited by the rapid recombination of photogenerated charge carriers and sluggish interfacial reaction kinetics. Herein, a hierarchically structured UiO-66-NH2(Hf) / ZnIn2S4 (denoted UN-66/ZIS) heterostructure was rationally fabricated via a solvothermal strategy to simultaneously regulate charge separation efficiency and optimize interfacial catalytic kinetics. Benefiting from the intimate heterointerface and built-in electric field, the optimized UN-66/ZIS sample exhibits remarkably improved visible-light absorption capability and charge transport efficiency, achieving a photocatalytic hydrogen production of 6052 ± 206 μmol·g-1, which greatly outperforms pristine UN-66 and ZIS. More importantly, in-situ X-ray photoelectron spectroscopy combined with density functional theory calculations directly unveils the mechanism of interfacial charge redistribution and directional electron transfer responsible for the enhanced carrier separation efficiency, offering mechanistic insights into the improved catalytic activity. Furthermore, loading of Pt cocatalyst effectively accelerates the surface hydrogen evolution kinetics. The corresponding hydrogen evolution rate increases to 14,403 ± 287 μmol·g-1·h-1, approximately seven times that of the Pt-free heterostructure. This work proposes a synergistic strategy integrating heterojunction engineering and cocatalyst modulation to simultaneously optimize light harvesting, charge separation and surface reaction kinetics, which provides new guidelines for the rational design of high-performance MOF/sulfide photocatalysts toward solar hydrogen production.
Tingting Yu, Yi-Qing Ran, Picheng Gong et al.· Journal of Colloid and Inter...· 0 citations
Spiramycin fermentation residues (SFR) are hazardous wastes enriched with residual antibiotics, yet they can serve as potential feedstocks for resource recovery after appropriate treatment. In this study, SFR-derived biochar (SFR-BC) was produced by pyrolysis and applied to agricultural soil to evaluate its effects on soil properties, microbial communities, potential pathogenic bacteria, antibiotic resistance genes (ARGs), and mobile genetic elements (MGEs). A 60-day soil incubation experiment was conducted with one control and three SFR-BC application rates of 0.5%, 1.0%, and 2.0%. SFR-BC improved soil physicochemical properties, nutrient status, enzyme activities, and microbial alpha diversity. Metagenomic analysis showed that SFR-BC altered the abundance of functional genes associated with carbon and nitrogen cycling, indicating shifts in microbial functional potential. SFR-BC also changed bacterial co-occurrence patterns, with the high-dose treatment showing a more complex and highly connected network structure during incubation. In addition, high-dose SFR-BC reduced several potential pathogenic bacteria, including major plant pathogenic taxa. SFR-BC decreased soil ARG abundance by 9.38%-33.67% and MGE abundance by 6.49%-27.89% relative to the control, showing a dose-dependent reduction in antibiotic resistance-related genetic elements. Network and PLS-PM analyses further indicated that ARG variation was statistically associated with soil physicochemical properties, microbial diversity, potential bacterial hosts, and MGEs. Overall, these results suggest that SFR-BC can improve short-term soil nutrient status and reduce ARGs, MGEs, and several potential pathogenic taxa under controlled incubation conditions, providing useful evidence for the potential valorization of antibiotic fermentation residues through pyrolysis.
Yepeng Tian, Jinzhi Sun, Quancheng Shu et al.· Bioresource Technology· 0 citations
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