Developing active, robust, and nonprecious electrocatalysts for the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR) is highly crucial and challenging. In this work, a facile strategy is developed for scalable fabrication of dicobalt phosphide (Co2P)–cobalt nitride (CoN) core–shell nanoparticles with double active sites encapsulated in nitrogen‐doped carbon nanotubes (Co2P/CoN‐in‐NCNTs) by straight forward pyrolysis method. Both density functional theory calculation and experimental results reveal that pyrrole nitrogen coupled with Co2P is the most active one for HER, while Co–N–C active sites existing on the interfaces between CoN and N‐doped carbon shells are responsible for the ORR and OER activity in this catalyst. Furthermore, liquid‐state and all‐solid‐state Zn–air batteries are equipped. Co2P/CoN‐in‐NCNTs show high power density as high as 194.6 mW cm−2, high gravimetric energy density of 844.5 W h kg−1, very low charge–discharge polarization, and excellent reversibility of 96 h at 5 mA cm−2 in liquid system. Moreover, the Co2P/CoN‐in‐NCNTs profiles confirm excellent activity for water splitting.
Structural and compositional engineering of atomic-scaled metal-N-C catalysts is important yet challenging in boosting their performance for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Here, boron (B)-doped Co-N-C active sites confined in hierarchical porous carbon sheets (denoted as Co-N,B-CSs) were obtained by a soft template self-assembly pyrolysis method. Significantly, the introduced B element gives an electron-deficient site that can activate the electron transfer around the Co-N-C sites, strengthen the interaction with oxygenated species, and thus accelerate reaction kinetics in the 4e processed ORR and OER. As a result, the catalyst showed Pt-like ORR performance with a half-wave potential (E) of 0.83 V versus (vs) RHE, a limiting current density of about 5.66 mA cm, and higher durability (almost no decay after 5000 cycles) than Pt/C catalysts. Moreover, a rechargeable Zn-air battery device comprising this Co-N,B-CSs catalyst shows superior performance with an open-circuit potential of ∼1.4 V, a peak power density of ∼100.4 mW cm, as well as excellent durability (128 cycles for 14 h of operation). DFT calculations further demonstrated that the coupling of Co-N active sites with B atoms prefers to adsorb an O molecule in side-on mode and accelerates ORR kinetics.
Bacteria, exemplified by enteropathogenic Escherichia coli (E. coli), rely on elaborate acid resistance systems to survive acidic environment (such as the stomach). Comprehensive understanding of bacterial acid resistance is important for prevention and clinical treatment. In this study, we report a previously uncharacterized type of acid resistance system in E. coli that relies on L-glutamine (Gln), one of the most abundant food-borne free amino acids. Upon uptake into E. coli, Gln is converted to L-glutamate (Glu) by the acid-activated glutaminase YbaS, with concomitant release of gaseous ammonia. The free ammonia neutralizes proton, resulting in elevated intracellular pH under acidic environment. We show that YbaS and the amino acid antiporter GadC, which exchanges extracellular Gln with intracellular Glu, together constitute an acid resistance system that is sufficient for E. coli survival under extremely acidic environment.
Halomonas bluephagenesis has been developed as a platform strain for the next generation industrial biotechnology (NGIB) with advantages of resistances to microbial contamination and high cell density growth (HCD), especially for production of polyhydroxyalkanoates (PHA) including poly(3-hydroxybutyrate) (PHB), poly(3-hydroxybutyrate-co-4-hydroxybutyrate) (P34HB) and poly(3-hydroxybutyrate-co-3-hydroxyvalerate) (PHBV). However, little is known about the mechanism behind PHA accumulation under oxygen limitation. This study for the first time found that H. bluephagenesis utilizes NADH instead of NADPH as a cofactor for PHB production, thus revealing the rare situation of enhanced PHA accumulation under oxygen limitation. To increase NADH/NAD ratio for enhanced PHA accumulation under oxygen limitation, an electron transport pathway containing electron transfer flavoprotein subunits α and β encoded by etf operon was blocked to increase NADH supply, leading to 90% PHB accumulation in the cell dry weight (CDW) of H. bluephagenesis compared with 84% by the wild type. Acetic acid, a cost-effective carbon source, was used together with glucose to balance the redox state and reduce inhibition on pyruvate metabolism, resulting in 22% more CDW and 94% PHB accumulation. The cellular redox state changes induced by the addition of acetic acid increased 3HV ratio in its copolymer PHBV from 4% to 8%, 4HB in its copolymer P34HB from 8% to 12%, respectively, by engineered H. bluephagenesis. The strategy of systematically modulation on the redox potential of H. bluephagenesis led to enhanced PHA accumulation and controllable monomer ratios in PHA copolymers under oxygen limitation, reducing energy consumption and scale-up complexity.
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