Interfacial Synergy of Cation Enrichment and Hydrophobicity in Bi2S3 Nanoflowers for Efficient Acidic CO2 Electroreduction.

IF 9.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2025-09-29 DOI:10.1021/acs.nanolett.5c02622

Weizhou Wang,Xuhua Zhao,Tian Dong,Yanling Geng,Zexing Wu,Jianping Lai,Bin Li,Hongdong Li,Lei Wang

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Abstract

The implementation of acidic CO2 electroreduction (CO2RR) is hindered by catalyst corrosion and the parasitic hydrogen evolution reaction (HER). We construct a hydrophobic hexadecyltrimethoxysilane (HDTMS)-modified Bi2S3 nanoflower catalyst (Bi2S3-C16) synergistically integrating cationic enrichment and interfacial hydrophobicity to achieve stable CO2-to-HCOOH conversion at pH = 2. COMSOL simulations reveal that the high-curvature architecture amplifies local electric fields, driving K+ accumulation to stabilize *OCHO intermediates via dipole interactions. The density functional theory also confirms this, showing a reduced *CO2→*OCHO energy barrier. In situ ATR-FTIR captures *OCHO vibrational modes (1575 cm-1) and HCOOH signatures (1695 cm-1). HDTMS reduces proton accessibility (rotating disc electrode analysis), suppressing HER. Consequently, Bi2S3-C16 achieves 89.6% HCOOH Faradaic efficiency at -400 mA cm-2 with 44.46% cathodic energy efficiency, operating stably for 48 h. This provides a paradigm for interfacial microenvironment control in harsh electrocatalytic systems.

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Bi2S3纳米花中阳离子富集和疏水性的界面协同作用用于高效的酸性CO2电还原。

酸性CO2电还原（CO2RR）的实现受到催化剂腐蚀和寄生析氢反应（HER）的阻碍。我们构建了一种疏水十六烷基三甲氧基硅烷（HDTMS）修饰的Bi2S3纳米花催化剂（Bi2S3- c16），将阳离子富集和界面疏水性协同结合，在pH = 2时实现了稳定的co2 - hcooh转化。COMSOL模拟表明，高曲率结构放大了局部电场，通过偶极子相互作用驱动K+积累以稳定*OCHO中间体。密度泛函理论也证实了这一点，显示出降低的*CO2→*OCHO能量势垒。原位ATR-FTIR捕获*OCHO振动模式（1575 cm-1）和HCOOH特征（1695 cm-1）。HDTMS降低质子可及性（旋转圆盘电极分析），抑制HER。因此，Bi2S3-C16在-400 mA cm-2下达到89.6%的HCOOH法拉第效率，阴极能量效率为44.46%，稳定运行48小时。这为恶劣电催化系统中的界面微环境控制提供了范例。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

期刊介绍： Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.