Engineering heterojunction is an underlying strategy to develop remarkable electrocatalysts for carbon dioxide (CO₂) reduction due to its ability to tune electronic properties by interfacial cooperation. Herein, we report a novel type of cube-like Zn₂SnO₄/SnO₂ heterostructure catalyst for CO₂ reduction through a simple co-precipitation process. The high-quality heterostructures with band alignment promote interfacial charge transfer from Zn₂SnO₄ to SnO₂, achieving the electronic modulation of Zn₂SnO₄/SnO₂ for reducing the kinetic barriers of CO₂ reduction. Density functional theory further reveals that Zn₂SnO₄/SnO₂ allows HCOO* intermediate favorably stabilizing on its surface through improved hydrogen coverage effect comparing to pure Zn₂SnO₄ or SnO₂. The hybrid catalyst presents satisfactory CO₂ reduction properties with a stable HCOOH selectivity of 77% during 24 h at −1.08 V vs. RHE. This study provides a new heterostructure modeling and general methodology for electronic modulation and electrocatalysts development for high-performance CO₂ reduction.

工程异质结是一种开发卓越的电催化剂以减少二氧化碳（CO ₂）的潜在策略，这是由于其通过界面合作调节电子性能的能力。在这里，我们报告了一种新型的立方状Zn ₂ SnO ₄ / SnO ₂异质结构催化剂，可通过简单的共沉淀过程还原CO ₂。带隙取向的高质量异质结构促进了界面电荷从Zn ₂ SnO ₄转移到SnO ₂，实现了Zn ₂ SnO ₄ / SnO ₂的电子调制，从而降低了CO的动力学势垒。₂减少。密度泛函理论进一步表明，与纯Zn ₂ SnO ₄或SnO ₂相比，Zn ₂ SnO ₄ / SnO ₂可以通过改善的氢覆盖作用使HCOO *中间体在其表面上稳定地稳定。杂化催化剂表现出令人满意的CO ₂还原性能，在-1.08 V vs. RHE下的24小时内，HCOOH的稳定选择性为77％。这项研究提供了一种新的异质结构建模和通用方法，用于电子调制和电催化剂开发，以实现高性能的CO ₂还原。