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。

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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引用次数: 0

摘要

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。

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

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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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.