Ambient-Temperature Chlorobenzene Combustion by Ozone: Proton-Electron Concerted Polarization over Brønsted Acid/Single-Atom Ni Pairs on SmMn2O5.

Abstract

Low-temperature catalytic combustion of chlorinated volatile organic compounds (Cl-VOCs) is essential for atmospheric pollution control, as it minimizes the temperature-dependent formation of toxic byproducts. Herein, we present an innovative proton-electron concerted polarization method through constructing Brønsted acid (boric acid)/single-atom Ni pairs on SmMn2O5 (Ni/B-SMO), achieving unprecedented ozone (O3) activation efficiency for room-temperature chlorobenzene combustion. The synergistic interaction between Ni 3d and H 1s orbitals drives O3 polarization through the enhanced overlap with O 2p orbitals, which selectively promotes O3 heterolysis into singlet oxygen (1O2) rather than radicals, achieving 99.9% chlorobenzene conversion under near ambient conditions (30 °C, 0-3.2 vol % H2O) with complete suppression of toxic byproducts. Remarkably, the catalyst maintains exceptional stability due to the simultaneous water molecule activation at boron sites for hydrolytic dechlorination. This work provides fundamental insights into proton-electron concerted catalysis and establishes a new paradigm for designing energy-efficient environmental remediation technologies.