Ultrafast Hole Preservation with Undercoordinated Tungsten for Efficient Solar-to-Chemical Conversion

IF 19.3 1区 材料科学 Q1 CHEMISTRY, PHYSICAL ACS Energy Letters Pub Date : 2024-06-07 DOI:10.1021/acsenergylett.4c01336
Qiushi Hu, Shang Liu, Jingjing Liu, Meng Lin, Ruquan Ye, Xihan Chen
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Abstract

Solar-to-chemical conversion is crucial, as it can form chemicals that are easy to store. Hydrogen peroxide (H2O2) represents a favorable chemical for energy storage and disinfection. Solar driven H2O2 photocatalysis is a promising method, as it could greatly reduce costs and provide on-demand production. The big challenge lies in achieving optimum production rate with reasonable materials cost. Herein, by precise control of synthetic conditions, tungsten (W)-based metal–organic-framework (MOF) with up to 28.64% undercoordinated W4/5+ is prepared. The H2O2 photoproduction rate up to 330,000 μmol g–1 h–1 L–1 is achieved, highest for non-noble metal-based catalysts. A multistage solar driven evaporation system further increases H2O2 concentration to 0.43 wt %, reaching application level for water treatment. Such an efficient production originates from ultrafast hole preservation, which enables a two-electron transfer reaction pathway for H2O2 production. Our work highlighted the potential of MOF-based photocatalyst for on-demand and large scale H2O2 production.

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利用欠配位钨进行超快空穴保存,实现高效的太阳能-化学转换
太阳能转化为化学物质至关重要,因为它可以形成易于储存的化学物质。过氧化氢(H2O2)是一种有利于能源储存和消毒的化学物质。太阳能驱动的 H2O2 光催化是一种很有前景的方法,因为它可以大大降低成本,并提供按需生产。如何以合理的材料成本获得最佳生产率是一大挑战。在此,通过精确控制合成条件,制备出了钨 (W) 基金属有机框架 (MOF),其中 W4/5+ 的配位不足率高达 28.64%。该催化剂的 H2O2 光生成率高达 330,000 μmol g-1 h-1 L-1,是非贵金属基催化剂中最高的。多级太阳能驱动蒸发系统进一步将 H2O2 浓度提高到 0.43 wt %,达到了水处理的应用水平。如此高效的生产源于超快的空穴保存,从而实现了 H2O2 生产的双电子转移反应途径。我们的工作凸显了基于 MOF 的光催化剂按需大规模生产 H2O2 的潜力。
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来源期刊
ACS Energy Letters
ACS Energy Letters Energy-Renewable Energy, Sustainability and the Environment
CiteScore
31.20
自引率
5.00%
发文量
469
审稿时长
1 months
期刊介绍: ACS Energy Letters is a monthly journal that publishes papers reporting new scientific advances in energy research. The journal focuses on topics that are of interest to scientists working in the fundamental and applied sciences. Rapid publication is a central criterion for acceptance, and the journal is known for its quick publication times, with an average of 4-6 weeks from submission to web publication in As Soon As Publishable format. ACS Energy Letters is ranked as the number one journal in the Web of Science Electrochemistry category. It also ranks within the top 10 journals for Physical Chemistry, Energy & Fuels, and Nanoscience & Nanotechnology. The journal offers several types of articles, including Letters, Energy Express, Perspectives, Reviews, Editorials, Viewpoints and Energy Focus. Additionally, authors have the option to submit videos that summarize or support the information presented in a Perspective or Review article, which can be highlighted on the journal's website. ACS Energy Letters is abstracted and indexed in Chemical Abstracts Service/SciFinder, EBSCO-summon, PubMed, Web of Science, Scopus and Portico.
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