Efficient photocatalytic CO2 Reduction to C2+ Products with Pt1-xPdxSn4 Dirac Nodal Arc Semimetal

TL;DR

This study introduces a novel Dirac nodal arc semimetal catalyst with optimized electronic structure that significantly improves selectivity and efficiency in photocatalytic CO2 reduction to C2+ products.

Contribution

It demonstrates how strategic Pt incorporation into PdSn4 enhances electronic properties and catalytic performance for CO2 reduction, establishing a new design paradigm for photocatalysts.

Findings

Achieved 73.1% product selectivity for C2H4.

Enhanced carrier mobility by 40% compared to pristine PdSn4.

Realized a C2H4 formation rate of 0.000328 mol g-1 h-1.

Abstract

The photochemical CO2 reduction reaction represents a zero-carbon pathway for converting CO2 into value-added chemicals, yet its industrial implementation has been constrained by low selectivity and product diversity. Dirac nodal arc semimetals characterized by ultrahigh carrier mobility with over 25000 cm2 V-1 s-1 offer a promising platform to search for efficient catalysts for CO2 conversion. Herein, we demonstrate that strategic Pt incorporation into PdSn4 optimizes the electronic structure and carrier dynamics of this Dirac semimetal. Experimental and theoretical analyses reveal that the resulting Pd-Sn-Pt local electronic structure redistributes charge density around Pd and Pt atoms, which facilitates C-C coupling via *OC-COH and *OC-CHOH intermediates and enhances carrier mobility by 40% versus the pristine PdSn4 single crystal. The optimized Pd0.4Pt0.6Sn4 single crystal achieves C2H4 with formation rate of 0.000328 mol g-1 h-1, product selectivity of 73.1% and electron-based selectivity of 89%. This work establishes electronic-structure-tunable Dirac semimetals as a new paradigm for multi-carbon photochemical CO2 reduction, providing a design strategy for next-generation photocatalysts.