Li Junhua,Jiang Yi,Zhang Xu,Huo Yidan,Du Fanglin,Tuo Yongxiao,Guo Zhiyan,Chen Dawei,Chen Shenghua
The electrooxidation of the alcohol and aldehyde molecules instead of water coupled with H 2 production has been proven to be effective for producing high-value fine chemicals under alkaline conditions. It is also noteworthy that under acidic conditions, the stability of non-noble metal water oxidation catalysts remains a great challenge due to the lattice oxygen mechanism. Hence, we coupled the biomass-derived glucose oxidation for high-value D-glucaric acid (GRA) with ultra-durable hydrogen in acid solution over a Yb-MnO 2 catalyst. The Mn 3+ regulated by Yb atoms doped in MnO 2 can effectively optimize the adsorption and desorption processes of the alcohol and aldehyde group and improve the intrinsic activity but cannot for H 2 O. The catalyst exhibited extremely high activity and stability after 50 h for glucose oxidation, inhibiting the lattice oxygen process and MnO 4− formation, while the activity was quickly lost within 0.5 h for water oxidation. Density functional theory (DFT) calculations further demonstrated that glucose oxidation reaction proceeds preferentially due to the oxidation of aldehyde group with lower adsorption-free energy (−0.4 eV) than water (Δ G > 0 eV), avoiding the lattice oxygen mechanism. This work suggests that biomass-derived glucose oxidation not only provides a cost-effective approach for high-value chemicals, but also shows an extremely potential as an alternative to acidic oxygen evolution reaction (OER) for ultradurable H 2 production.
Pharmaceuticals and personal care products (PPCPs), known for their severe ecological risks, are frequently detected in coastal waters worldwide. However, the environmental fate in marine systems remains poorly understood. This study investigated the co-metabolic degradation mechanism of a typical PPCP, sulfamethoxazole (SMX), by a marine consortium SAB using alginate—a natural organic matter—as a co-substrate, aiming to elucidate the biodegradation process of PPCPs in actual marine environments. An integrated approach, including metagenomic sequencing (with binning), RT-qPCR, molecular docking, metabolic modeling, and metabolomics, was employed. Results demonstrated that the SAB consortium efficiently degraded SMX at concentrations from 50 μg/L to 10 mg/L, achieving over 96% removal within 24 h. SMX degradation was achieved through metabolic cross-feeding of alginate by key species within the SAB consortium. Specifically, alginate is initially converted by Vibrio into the central metabolite 2-keto-3-deoxy-D-gluconate (KDG). KDG is subsequently metabolized by Tritonibacter , Halopseudomonas , and Vibrio , generating key metabolites such as acetyl-CoA, serine, cysteine, and guanine. These metabolites support microbial growth and induce production of SMX-degrading enzymes, such as threonine dehydratase, cysteine S-conjugate β-lyase, and guanine deaminase, leading to SMX cleavage and mineralization. Additionally, acetyl-CoA provides acetyl groups for arylamine N-acetyltransferase-mediated SMX acetylation. These processes collectively drive the co-metabolic degradation of SMX. Overall, this study provides critical insights into PPCPs' fate in marine environments.
危险品化学品经营许可证（带存储）