Al-N<sub>3</sub> Bridge Site Enabling Interlayer Charge Transfer Boosts the Direct Photosynthesis of Hydrogen Peroxide from Water and Air

doi:10.1021/jacs.4c11471

IMR OpenIR

	Al-N₃ Bridge Site Enabling Interlayer Charge Transfer Boosts the Direct Photosynthesis of Hydrogen Peroxide from Water and Air
	Tan, Hao 1,2; Zhou, Peng 3; Liu, Meixian 4; Gu, Yu 1; Chen, Wenxing 5; Guo, Hongyu 1; Zhang, Jiankang 6; Yin, Kun 1; Zhou, Yin 1; Shang, Changshuai 1; Zhang, Qinghua 7; Gu, Lin 7; Zhang, Nian 8; Ma, Jingyuan 8; Zheng, Zhanfeng 4; Luo, Mingchuan 1,9; Guo, Shaojun 1,9
通讯作者	Guo, Shaojun(guosj@pku.edu.cn)
	2024-11-05
发表期刊	JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
ISSN	0002-7863
卷号	146 期号:46 页码:31950-31960
摘要	Manipulating the electronic environment of the reactive center to lower the energy barrier of the rate-determining water oxidation step for boosting the direct generation of H2O2 from water, air, and sunlight is fascinating yet remains a grand challenge. Driven by a first-principles screening across a series of metal single atoms in carbon nitride, we report a class of an Al-N3 bridge site enabling interlayer charge transfer in carbon nitride nanotubes (CNNT-Al) for the highly efficient photosynthesis of H2O2 directly from water, oxygen, and sunlight. We demonstrate that the interlayered Al-N3 bridge site in CNNT-Al is able to activate the neighboring surface N atom for promoting the rate-determining step of the two-electron water oxidation to H2O2. It is also able to act as a bridge for enhancing the vertical interlaminar charge transfer due to the hybridization between the 3s and 3p states of the interstitial Al atom and the conduction band of two adjacent carbon nitride layers. Collectively, these factors lead to a highest photocatalytic mass activity of 1410.2 mu mol g-1 h-1 (with a photocatalyst concentration of 1 g L-1) for direct photosynthesis of H2O2 out of all CN-based photocatalysts and a 7-fold higher solar-to-chemical conversion efficiency (0.73%) compared to that of the natural photosynthesis of typical plants (similar to 0.1%). Most importantly, the CNNT-Al-based flow reactor can steadily produce H2O2 for 200 h and be directly used for the on-site degradation of organic dye in water. The CNNT-Al-based flow reactor can also kill a 10 times higher concentration of bacteria in deionized water than that in natural water with 100% efficiency, which makes our design economically appealing for practical water treatment.
资助者	National Key R&D Program of China ; National Science Fund for Distinguished Young Scholars ; Beijing Natural Science Foundation ; Tencent Foundation through the XPLORER PRIZE ; National Natural Science Foundation of China
DOI	10.1021/jacs.4c11471
收录类别	SCI
语种	英语
资助项目	National Key R&D Program of China[2022YFE0128500] ; National Science Fund for Distinguished Young Scholars[52025133] ; Beijing Natural Science Foundation[Z220020] ; Tencent Foundation through the XPLORER PRIZE ; National Natural Science Foundation of China[22309005] ; National Natural Science Foundation of China[2230906]
WOS研究方向	Chemistry
WOS类目	Chemistry, Multidisciplinary
WOS记录号	WOS:001349081000001
出版者	AMER CHEMICAL SOC
引用统计	被引频次：2[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/191219
专题	中国科学院金属研究所
通讯作者	Guo, Shaojun
作者单位	1.Peking Univ, Sch Mat Sci & Engn, Beijing 100871, Peoples R China 2.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 3.Peking Univ, Shenzhen Grad Sch, Sch Environm & Energy, Shenzhen 518055, Peoples R China 4.Chinese Acad Sci, State Key Lab Coal Convers, Inst Coal Chem, Taiyuan 030001, Peoples R China 5.Beijing Inst Technol, Energy & Catalysis Ctr, Sch Mat Sci & Engn, Beijing 100081, Peoples R China 6.Northwestern Polytech Univ, Interdisciplinary Res Ctr Biol & Catalysis, Sch Life Sci, Xian 710072, Peoples R China 7.Chinese Acad Sci, Inst Phys, Beijing 100871, Peoples R China 8.Chinese Acad Sci, Shanghai Synchrotron Radiat Facil, Shanghai Inst Appl Phys, Shanghai 201204, Peoples R China 9.Peking Univ, Beijing Innovat Ctr Engn Sci & Adv Technol, Beijing 100871, Peoples R China
推荐引用方式 GB/T 7714	Tan, Hao,Zhou, Peng,Liu, Meixian,et al. Al-N₃ Bridge Site Enabling Interlayer Charge Transfer Boosts the Direct Photosynthesis of Hydrogen Peroxide from Water and Air[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2024,146(46):31950-31960.
APA	Tan, Hao.,Zhou, Peng.,Liu, Meixian.,Gu, Yu.,Chen, Wenxing.,...&Guo, Shaojun.(2024).Al-N₃ Bridge Site Enabling Interlayer Charge Transfer Boosts the Direct Photosynthesis of Hydrogen Peroxide from Water and Air.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,146(46),31950-31960.
MLA	Tan, Hao,et al."Al-N₃ Bridge Site Enabling Interlayer Charge Transfer Boosts the Direct Photosynthesis of Hydrogen Peroxide from Water and Air".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 146.46(2024):31950-31960.