不对称原子Pt-B双址催化剂在海水中高效光重整废聚乳酸塑料

IF 15.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
ACS Nano Pub Date : 2025-04-18 DOI:10.1021/acsnano.5c02408
Zongyang Ya, Mei Li, Dong Xu, Hua Wang, Shengbo Zhang
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引用次数: 0

摘要

废塑料给海洋生态系统带来了巨大的负担。通过光催化将塑料转化为高价值产品是一种新兴的、有前途的方法,但其低活性和产品选择性带来了很大的挑战。在此,我们报道了一种氮化碳锚定的原子分散Pt - b双位点催化剂(Pt SA/BCN100),用于在海水中光重整聚乳酸(PLA)为高价值化学品和H2。实验和DFT计算表明,Pt位点和B位点之间的电荷转移显著增强,富空穴的B位点可以选择性地触发PLA的C-H和C-C键的激活和裂解形成乙酸(AA),而富电子的Pt位点则驱动H质子还原成H2。结果表明,Pt SA/BCN100具有993 μmol gcatal-1 h-1的H2生成速率和300 μmol gcatal-1 h-1的AA生成速率,选择性超过98%。我们还展示了在天然海水中直接光重整g级真实聚乳酸废物和低浓度聚乳酸微塑料。技术经济分析和环境评价表明,该催化体系可显著降低碳排放,具有潜在的商业价值。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Asymmetric Atomic Pt–B Dual-Site Catalyst for Efficient Photoreforming of Waste Polylactic Acid Plastics in Seawater

Asymmetric Atomic Pt–B Dual-Site Catalyst for Efficient Photoreforming of Waste Polylactic Acid Plastics in Seawater
Waste plastic has imposed significant burdens on marine ecosystems. Converting plastic into high-value products via photocatalysis is an emerging and promising approach, but its low activity and product selectivity pose great challenges. Herein, we report a carbon nitride-anchored atomically dispersed Pt–B dual-site catalyst (Pt SA/BCN100) for the photoreforming of polylactic acid (PLA) into high-value chemicals and H2 in seawater. Experiments and DFT calculations reveal that significantly enhanced charge transfer occurs between the Pt site and the B site, and the hole-rich B site can selectively trigger the activation and cleavage of the C–H and C–C bonds of PLA to form acetic acid (AA), while the electron-rich Pt site drives the reduction of H protons to H2. As a result, Pt SA/BCN100 exhibits a high H2 evolution rate of 993 μmol gcatal–1 h–1 and an AA production rate of 300 μmol gcatal–1 h–1 with a selectivity of over 98%. We also demonstrate the direct photoreforming of g-scale real-world PLA wastes and low concentrations of PLA microplastics in natural seawater. Techno-economic analysis and environmental assessment show that this catalytic system can significantly reduce carbon emissions and has potential commercial value.
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来源期刊
ACS Nano
ACS Nano 工程技术-材料科学:综合
CiteScore
26.00
自引率
4.10%
发文量
1627
审稿时长
1.7 months
期刊介绍: ACS Nano, published monthly, serves as an international forum for comprehensive articles on nanoscience and nanotechnology research at the intersections of chemistry, biology, materials science, physics, and engineering. The journal fosters communication among scientists in these communities, facilitating collaboration, new research opportunities, and advancements through discoveries. ACS Nano covers synthesis, assembly, characterization, theory, and simulation of nanostructures, nanobiotechnology, nanofabrication, methods and tools for nanoscience and nanotechnology, and self- and directed-assembly. Alongside original research articles, it offers thorough reviews, perspectives on cutting-edge research, and discussions envisioning the future of nanoscience and nanotechnology.
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