Atomically-thin Schottky-like photo-electrocatalytic cross-flow membrane reactors for ultrafast remediation of persistent organic pollutants

Abstract

The remediation of persistent organic pollutants in surface and ground water represents a major environmental challenge worldwide. Conventional physico-chemical techniques do not efficiently remove such persistent organic pollutants and new remediation techniques are therefore required. Photo-electro catalytic membranes represent an emerging solution that can combine photocatalytic and electrocatalytic degradation of contaminants along with molecular sieving. Herein, macro-porous photo-electro catalytic membranes were prepared using conductive and porous stainless steel metal membranes decorated with nano coatings of semiconductor photocatalytic metal oxides (TiO₂ and ZnO) via atomic layer deposition, producing highly conformal and stable coatings. The metal - semiconductor junction between the stainless steel membranes and photocatalysts provides Schottky - like characteristics to the coated membranes. The PEC membranes showed induced hydrophilicity from the nano-coatings and enhanced electro-chemical properties due to the Schottky junction. A high electron transfer rate was also induced in the coated membranes as the photocurrent efficiency increased by 4 times. The photo-electrocatalytic efficiency of the TiO₂ and ZnO coated membranes were demonstrated in batch and cross flow filtration reactors for the degradation of persistent organic pollutant solution, offering increased degradation kinetic factors by 2.9 and 2.3 compared to photocatalysis and electrocatalysis, respectively. The recombination of photo-induced electron and hole pairs is mitigated during the photo-electrocatalytic process, resulting in an enhanced catalytic performance. The strategy offers outstanding perspectives to design stimuli-responsive membrane materials able to sieve and degrade simultaneously toxic contaminants towards greater process integration and self-cleaning operations.

Keywords: Atomic layer deposition; Membrane catalytic reactor; Persistent organic pollutants; Photo-electrocatalysis; Schottky-like diodes.