Oxygen Functional Groups Regulate Cobalt-Porphyrin Molecular Electrocatalyst for Acidic H2O2 Electrosynthesis at Industrial-Level Current.

Electrosynthesis of hydrogen peroxide (H2O2) based on proton exchange membrane (PEM) reactor represents a promising approach to industrial-level H2O2 production, while it is hampered by the lack of high-efficiency electrocatalysts in acidic medium. Herein, we present a strategy for the specific oxygen functional group (OFG) regulation to promote the H2O2 selectivity up to 92% in acid on cobalt-porphyrin molecular assembled with reduced graphene oxide. In-situ X-ray adsorption spectroscopy, in-situ Raman spectroscopy and Kelvin probe force microscopy combined with theoretical calculation unravel that different OFGs exert distinctive regulation effects on the electronic structure of Co center through either remote (carboxyl and epoxy) or vicinal (hydroxyl) interaction manners, thus leading to the opposite influences on the promotion in 2e- ORR selectivity. As a consequence, the PEM electrolyzer integrated with the optimized catalyst can continuously and stably produce the high-concentration of ca. 7 wt% pure H2O2 aqueous solution at 400 mA cm-2 over 200 h with a cell voltage as low as ca. 2.1 V, suggesting the application potential in industrial-scale H2O2 electrosynthesis.

Crystalline Phase Engineering to Modulate the Interfacial Interaction of the Ruthenium/Molybdenum Carbide for Acidic Hydrogen Evolution.

Ruthenium (Ru) is an ideal substitute to commercial Pt/C for the acidic hydrogen evolution reaction (HER), but it still suffers from undesirable activity due to the strong adsorption free energy of H* (ΔGH*). Herein, we propose crystalline phase engineering by loading Ru clusters on precisely prepared cubic and hexagonal molybdenum carbide (α-MoC/ß-Mo2C) supports to modulate the interfacial interactions and achieve high HER activity. Advanced spectroscopies demonstrate that Ru on ß-Mo2C shows a lower valence state and withdraws more electrons from the support than that of Ru on α-MoC, indicative of a strong interfacial interaction. Density functional theory reveals that the ΔGH* of Ru/ß-Mo2C approaches 0 eV, illuminating an enhancement mechanism at the Ru/ß-Mo2C interface. The resultant Ru/ß-Mo2C exhibits an encouraging performance in a proton exchange membrane water electrolyzer with a low cell voltage (1.58 V@ 1.0 A cm-2) and long stability (500 h@ 1.0 A cm-2).

Biodegradable and multifunctional black mulch film decorated with darkened lignin induced by iron ions for "green" agriculture.

High-value utilization of bleached lignin has been widely used in different fields, whereas the investigation on darkened lignin in composite materials was often ignored. In this work, a sort of eco-friendly and structurally robust sodium carboxymethyl cellulose (CMC)/polyvinyl alcohol (PVA)/sodium lignosulfonate (SLS) black composite mulch film was elaborately designed. The chelation and redox reaction effect between Fe ions and SLS lead to the formation of a more quinones structure on lignin, darkening both lignin and the mulch films. The chelation effect between Fe ions and biopolymer formed three-dimensional structures, which can be used as sacrifice bonds to dissipate energy and improve the mechanical properties of the composite films. In particular, the maximum elongation at break and toughness increased from 48.4 % and 1141 kJ/m3 for the CMC/PVA film to 210.9 % and 1426 kJ/m3 for the optimized CMC/PVA/SLS/Fe black mulch film, respectively. In addition, the optimized black mulch film also possesses good soil water retention, thermal preservation effect, controlled urea release, and well biodegradability. This work offered a novel strategy for designing eco-friendly black mulch with reinforced mechanical strength, slow-release urea, soil moisture retention, and heat preservation performances.

Different responses of taxonomic and functional trait structure of benthic macroinvertebrate assemblages to eutrophication in a large Chinese freshwater lake.

Functional trait measures have the potential to represent local habitat conditions and are considered promising tools for biomonitoring and bioassessment programs. Macroinvertebrates are an ecologically significant group in freshwater ecosystems and possess a range of functional traits which are employed to assess ecological quality. Nevertheless, the relationships between macroinvertebrate functional structure and anthropogenic disturbances remain poorly understood. In this study, we conducted a comparison of how functional trait-based and taxonomy-based composition of macroinvertebrate assemblages responded to eutrophication in Lake Taihu, a typical large eutrophic freshwater lake in China. Specifically, we examined both the taxonomy-based and trait-based compositions of benthic macroinvertebrates varied along the eutrophication gradient. Eutrophication was associated with remarkable decreases in the abundance of gastropod taxa and increases in Oligochaeta and Chironomidae. Ten categories belonging to six traits were significantly different among three site groups. The eutrophic and transition sites showed higher abundance of Size2, burrowers, and integument-respiration organisms than macrophytic sites, whereas abundance of Size1, conical-shaped, sprawlers, scrapers, and lung-respiration were higher in macrophytic sites. Both taxonomic (36.8%) and functional compositions (39.8%) of macroinvertebrate assemblages were influenced by the same variables: CODMn and transparency. Our study showed that macroinvertebrate trait-based approaches can be considered a useful supplement to traditional taxonomic approach for biomonitoring programs in freshwater lakes.

Electrocatalytic water oxidation enabling the highly selective oxidation of styrene to benzaldehyde.

An electrooxidation strategy mediated by reactive oxygen species is proposed to realize the transformation of styrene to benzaldehyde on a Pt anode, with a high selectivity of ca. 89% and faradaic efficiency of 28.8%. Isotopic labelling, electron paramagnetic resonance and radical scavenging experiments revealed that OH˙ and O2-˙ species, formed in situ via anodic water oxidation, play a crucial role in the selective formation of benzaldehyde.