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基于八元高熵氧化物的可持续光催化过氧化氢生产

Sustainable photocatalytic hydrogen peroxide production over octonary high-entropy oxide.

作者信息

Ling Hao, Sun Huacong, Lu Lisha, Zhang Jingkun, Liao Lei, Wang Jianlin, Zhang Xiaowei, Lan Yingying, Li Renjie, Lu Wengang, Cai Lejuan, Bai Xuedong, Wang Wenlong

机构信息

Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, China.

School of Physical Sciences, University of Chinese Academy of Sciences, Chinese Academy of Sciences, Beijing, China.

出版信息

Nat Commun. 2024 Nov 3;15(1):9505. doi: 10.1038/s41467-024-53896-w.

Abstract

The direct utilization of solar energy for the artificial photosynthesis of hydrogen peroxide (HO) provides a reliable approach for producing this high-value green oxidant. Here we report on the utility of high-entropy oxide (HEO) semiconductor as an all-in-one photocatalyst for visible light-driven HO production directly from HO and atmospheric O without the need of any additional cocatalysts or sacrificial agents. This high-entropy photocatalyst contains eight earth-abundant metal elements (Ti/V/Cr/Nb/Mo/W/Al/Cu) homogeneously arranged within a single rutile phase, and the intrinsic chemical complexity along with the presence of a high density of oxygen vacancies endow high-entropy photocatalyst with distinct broadband light harvesting capability. An efficient HO production rate with an apparent quantum yield of 38.8% at 550 nm can be achieved. The high-entropy photocatalyst can be readily assembled into floating artificial leaves for sustained on-site production of HO from open water resources under natural sunlight irradiation.

摘要

直接利用太阳能进行过氧化氢(HO)的人工光合作用为生产这种高价值绿色氧化剂提供了一种可靠的方法。在此,我们报道了高熵氧化物(HEO)半导体作为一种一体化光催化剂的效用,该催化剂可直接利用HO和大气中的O在可见光驱动下生产HO,无需任何额外的助催化剂或牺牲剂。这种高熵光催化剂包含八个储量丰富的金属元素(Ti/V/Cr/Nb/Mo/W/Al/Cu)均匀排列在单一金红石相中,其内在的化学复杂性以及高密度氧空位的存在赋予了高熵光催化剂独特的宽带光捕获能力。在550 nm处可实现高效的HO产率,表观量子产率为38.8%。这种高熵光催化剂可以很容易地组装成漂浮人工叶片,以便在自然阳光照射下从开放水资源中持续现场生产HO。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/015e/11532407/b419e415db8b/41467_2024_53896_Fig1_HTML.jpg

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