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Title of Paper:Breaking the Limits of Piezo-Photocatalysis: Pd-O D-p Orbital Hybridization Mediated Charge Reconstruction and Polarization Enhancement

Journal:Advanced Functional Materials

Place of Publication:Wiley

Key Words:piezo-photocatalyst, d-p orbital hybridization, charge asymmetry, sulfur vacancy, 2,4-dichlorophenol, H2O2

Summary:Piezo-photocatalysis have emerged as a promising strategy to suppress charge recombination in conventional photocatalysis for removal of refractory organic pollutants and green hydrogen peroxide (H2O2) production. Nevertheless, sulfide-based piezo-photocatalysts still suffer from weak piezoelectric response and ambiguous coupling mechanisms between atomic orbitals and polarization. Herein, we designed Pd-doped and lattice oxygen-modified Zn3In2S6 piezo-photocatalyst (Zn3In2S6-Pd-350) by regulating d-p orbital hybridization at Pd sites to achieve efficient piezo-photocatalytic performance. Lattice oxygen occupies sulfur vacancies and converts Pd–S into Pd–O coordination, enabling strong Pd 4d–O 2p orbital hybridization. The σ* and π* antibonding orbitals act as electron acceptors to accelerate charge separation. The charge asymmetry induced by Pd and lattice oxygen enhanced piezoelectric properties of catalyst, resulting in a 156% increase of the piezoelectric coefficient. Zn3In2S6-Pd-350 achieved 100% degradation of 2,4-DCP and H2O2 yield of 327.9 µmol·g-1·h-1, accompanied by •OH, •O2⁻ and ¹O2 synergistic oxidation. Calculations confirm that single-atom Pd replacing Zn is the active center with optimal Pd–S1O3 coordination, and external strain further enhances O2/H2O adsorption. This work establishes an atomic-level design strategy via orbital engineering, reveals the essential synergy among orbital hybridization, charge distribution and piezoelectric polarization, and provides a feasible route for chlorophenol wastewater remediation and low-carbon H2O2 synthesis.

First Author:Meng Dai

Correspondence Author:Zuoli He

All the Authors:Yi Ren,Shumeng Qin,Hongsheng Li,Ziye Zheng,Lihui Xiao,Dong Zhai,Xiaoge Wu,Shuguang Wang

Indexed by:Journal paper

Document Code:79377

Discipline:Engineering

First-Level Discipline:Environmental Science and Engineering

Document Type:J

Page Number:79377

DOI Number:10.1002/adfm.79377

Number of Words:9259

Translation or Not:No

Date of Publication:2026-10

Included Journals:SCI

Release Time:2026-10-27