Integrating Hydrogen Production and Transfer Hydrogenation with Selenite Promoted Electrooxidation of α‐Nitrotoluenes to E‐Nitroethenes

Abstract

Developing an electrochemical carbon‐added reaction with accelerated kinetics to replace the low‐value and sluggish oxygen evolution reaction (OER) is markedly significant to pure hydrogen production. Regulating the critical steps to precisely design electrode materials to selectively synthesize targeted compounds is highly desirable. Here, inspired by the surfaced adsorbed SeOx2− promoting OER, NiSe is demonstrated to be an efficient anode enabling α‐nitrotoluene electrooxidation to E‐nitroethene with up to 99 % E selectivity, 89 % Faradaic efficiency, and the reaction rate of 0.25 mmol cm−2 h−1 via inhibiting side reactions for energy‐saving hydrogen generation. The high performance can be associated with its in situ formed NiOOH surface layer and absorbed SeOx2− via Se leaching‐oxidation during electrooxidation, and the preferential adsorption of two ‐NO2 groups of intermediate on NiOOH. A self‐coupling of α‐carbon radicals and subsequent elimination of a nitrite molecule pathway is proposed. Wide substrate scope, scale‐up synthesis of E‐nitroethene, and paired productions of E‐nitroethene and hydrogen or N‐protected aminoarenes over a bifunctional NiSe electrode highlight the promising potential. Gold also displays a similar promoting effect for α‐nitrotoluene transformation like SeOx2−, rationalizing the strategy of designing materials to suppress side reactions.

Promoting water dissociation for efficient solar driven CO2 electroreduction via improving hydroxyl adsorption

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Nitrogen, Phosphorus, and Sulfur Tri-doped Carbon A Coated NiCo2Se4 Needle Arrays Grown on Carbon Cloth as Binder-free Anode for Potassium-Ion Batteries

“…In Figure 3E, the peaks at 55.6 and 54.7 eV correspond to the spin-orbit peaks of Se 3d 3/2 and Se 3d 5/2 . A broad peak at 59.4 eV can be related to the SeO x (Chong et al, 2021). The C 1s high-resolution XPS spectrum is depicted in Figure 3F, which can be fitted into four peaks including C-C/C=C (284.4 eV), C-N or C-S (285.9 eV), C-P (287.1 eV), and O=C-O (290.1 eV).…”

An Electrocatalytic Strategy for Dehydrogenative [4 + 2] Cycloaddition over a Cobalt‐Based Catalyst

“…We then investigated the electrocatalytic performance over the as‐synthesized CCHH‐A/CC under the optimized conditions. The linear sweep voltammetry (LSV) curves (Figure 3a) display an obvious increase in current density after the addition of 1a and 2a , [ 23 ] indicating the occurrence of electrochemical oxidation. The required potential for gaining current density of 10 mA·cm –2 dramatically decreased from 1.76 V to 1.16 V vs. Ag/AgCl.…”