Electrocatalytic Hydrodechlorination Using Supported Atomically Precise Gold Nanoclusters under Flow-Through Configuration

Abstract

We developed and optimized an electrocatalytic filtration system to catalytically hydrodechlorinate chlorophenolic compounds. A key part of the system was the cathode, which consisted of a filter constructed with electroactive carbon nanotubes (CNTs) functionalized with atomically precise gold nanoclusters (AuNCs). In the functional membrane electrode, the AuNCs attached to the CNTs functioned as a highly effective hydrodechlorination catalyst. Additionally, the ligands of the AuNCs facilitated the binding of the AuNCs with the CNT and protected the Au core from agglomeration. Atomic H* was the primary reactive species in the system, but direct reduction by cathode electrons also contributed to the elimination of 2,4-dichlorophenol (2,4-DCP) by hydrodechlorination. The generated atomic H* was able to break the C–Cl bond to achieve the rapid hydrodechlorination of 2,4-DCP into phenol, with 91.5% 2,4-DCP removal within 120 min. The AuNC catalysts attached to the CNT exceeded the best catalytic activity of larger nanoparticles (e.g., AuNPs), while the flow-through construction performed better than a standard batch reactor due to the convection-enhanced mass transport. The study provides an environmentally friendly strategy for the elimination of pervasive halogenated organic contaminants using a highly efficient, stable and recyclable system for hydrodechlorination that integrates nanofiltration and electrochemistry.