Hydrogenation of Nitroarenes by Onsite-Generated Surface Hydroxyl from Water

Directly using water as a hydrogen source for hydrogenation of nitroarenes to anilines (HNA) without using H2 is an ideal reduction reaction route but is limited by unfavorable thermodynamics. Herein, we report a high-efficiency and durable H2O-based HNA process achieved by using in situ-generated hydroxyl species from water as a hydrogen donor and low-cost CO as an oxygen acceptor over a molybdenum carbide-supported gold catalyst (Au/α-MoC1–x). It affords nitroarene conversion of over 99% with aniline selectivity of over 99% and excellent functional group tolerance at 25 °C and remains stable after 10 cycles, outperforming the traditional H2-involved route. Spectroscopic and theoretical studies reveal the key role of Au/α-MoC1–x boundaries, at which not only hydroxyl species are generated as a soft reductant on α-MoC1–x but also the nitro group is selectively hydrogenated to anilines with other unsaturated groups intact, and residual O* is removed by adsorbed CO on the atomically thin Au layer. This process provides a durable H2O-based route for aniline production at room temperature

High-Pressure Electro-Fenton Driving CH₄ Conversion by O₂ at Room Temperature

Electrochemical conversion of CH4 to easily transportable and value-added liquid fuels is highly attractive for energy-efficient CH4 utilization, but it is challenging due to the low reactivity and solubility of CH4 in the electrolyte. Herein, we report a high-pressure electro-Fenton (HPEF) strategy to establish a hetero-homogeneous process for the electrocatalytic conversion of CH4 by O2 at room temperature. In combination with elevation of reactant pressure to accelerate reaction kinetics, it delivers an unprecedented HCOOH productivity of 11.5 mmol h–1 gFe–1 with 220 times enhancement compared to that under ambient pressure. Remarkably, an HCOOH Faradic efficiency of 81.4% can be achieved with an ultralow cathodic overpotential of 0.38 V. The elevated pressure not only promotes the electrocatalytic reduction of O2 to H2O2 but also increases the reaction collision probability between CH4 and •OH, which is in situ generated from the Fe2+-facilitated decomposition of H2O2

Efficiency scrutiny - have they listened? Third survey of Government policy towards the voluntary sector in Wales, 1993/94

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