Atomic Pt‐N₄ Sites in Porous N‐Doped Nanocarbons for Enhanced On‐Site Chlorination Coupled with H₂ Evolution in Acidic Water

Abstract

Acidic water electrolysis (AWE) has the potential to revolutionize green H2 generation with flexible partial load range, high gas purity, and rapid system response. However, the extensive usage of noble Ru/Ir metals and sluggish oxygen evolution reaction (OER) with inexpensive O2 products pose significant challenges in anodes. Herein, it is demonstrated that ultralow Pt single atoms in highly porous N‐doped carbons (Pt1/p‐NC@CNTs) can effectively catalyze chlorine evolution reaction (CER) for on‐site chlorination to replace OER in AWE, with 200 mV potential saving at 10 mA cm−2. As a result, various organic halide motifs of pharmaceutical molecules by chlorinating anisole, ketones, and olefins can be realized, along with H2 coproduction. Combined physicochemical characterizations including synchrotron X‐ray absorption spectroscopy, finite element methodsimulations, and theory calculations indicate that atomic Pt‐N4 active sites balance the adsorption/desorption of Cl intermediates (Volmer step) and the plentiful porosity of Pt1/p‐NC@CNTs with high specific surface area of 313 m2 g−1 enriches Cl− around active sites (Heyrovský step), collectively promoting the rate‐limiting Volmer–Heyrovský pathway for improved CER.

Water electrolysis for hydrogen production: from hybrid systems to self-powered/catalyzed devices

“…At present, the production of H 2 through water electrolysis is predominantly carried out using freshwater, which poses limitations in arid regions due to the scarcity of freshwater resources. 210 To address this, electrolysis of seawater for H 2 production has emerged as a promising alternative. However, the complex ionic environment of seawater presents challenges such as interference from anion side reactions and the corrosion of electrolyzers and catalysts.…”

Organocatalyst Supported by a Single‐Atom Support Accelerates both Electrodes used in the Chlor‐Alkali Industry via Modification of Non‐Covalent Interactions

“…Chlor‐alkali production is a vital source of daily chemicals for both personal and industrial use, including disinfectants and chlorine [1–8] . It is a significant pillar of the chemical industry, accounting for 2 % of global electricity generation, with an energy consumption of around 150 TW h y −1 .…”

Design Strategies towards Advanced Hydrogen Evolution Reaction Electrocatalysts at Large Current Densities

“…Hydrogen (H 2 ), with the fascinating properties including renewability, high gravimetric energy density, and zero‐emission of carbon dioxide, is an ideal energy carrier for the future world, and can be used to power fuel cell electric vehicles [1–3] . Besides the use in transportation sector, hydrogen is also an indispensable feedstock for some important industrial processes such as oil refining, ammonia synthesis, methanol production, etc [4] .…”