Integration of bio-inspired lanthanide-transition metal cluster and P-doped carbon nitride for efficient photocatalytic overall water splitting

被引：27

作者：

Chen, Rong ^{[1
,2
]}

Zhuang, Gui-Lin ^{[3
]}

Wang, Zhi-Ye ^{[1
,2
]}

Gao, Yi-Jing ^{[3
]}

Li, Zhe ^{[1
,2
]}

Wang, Cheng ^{[1
,2
]}

Zhou, Yang ^{[1
,2
]}

Du, Ming-Hao ^{[1
,2
]}

Zeng, Suyuan ^{[4
]}

Long, La-Sheng ^{[1
,2
]}

Kong, Xiang-Jian ^{[1
,2
]}

Zheng, Lan-Sun ^{[1
,2
]}

机构：

[1] Xiamen Univ, Coll Chem & Chem Engn, Collaborat Innovat Ctr Chem Energy Mat, State Key Lab Phys Chem Solid Surface, Xiamen 361005, Peoples R China

[2] Xiamen Univ, Coll Chem & Chem Engn, Dept Chem, Xiamen 361005, Peoples R China

[3] Zhejiang Univ Technol, Coll Chem Engn, Hangzhou 310032, Peoples R China

[4] Liaocheng Univ, Coll Chem & Chem Engn, Liaocheng 252059, Shandong, Peoples R China

来源：

NATIONAL SCIENCE REVIEW | 2021年 / 8卷 / 09期

基金：

中国国家自然科学基金;

关键词：

bio-inspired; lanthanide-transition metal cluster; photocatalytic overall water splitting; synergistic effects; oxygen-evolving center; OXYGEN-EVOLVING COMPLEX; PHOTOSYSTEM-II; OXIDATION; CO4O4; NANOSHEETS; CATALYST; CLOSER;

D O I：

10.1093/nsr/nwaa234

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Photosynthesis in nature uses the Mn4CaO5 cluster as the oxygen-evolving center to catalyze the water oxidation efficiently in photosystem II. Herein, we demonstrate bio-inspired heterometallic LnCo(3) (Ln = Nd, Eu and Ce) clusters, which can be viewed as synthetic analogs of the CaMn4O5 cluster. Anchoring LnCo(3) on phosphorus-doped graphitic carbon nitrides (PCN) shows efficient overall water splitting without any sacrificial reagents. The NdCo3/PCN-c photocatalyst exhibits excellent water splitting activity and a quantum efficiency of 2.0% at 350 nm. Ultrafast transient absorption spectroscopy revealed the transfer of a photoexcited electron and hole into the PCN and LnCo(3) for hydrogen and oxygen evolution reactions, respectively. A density functional theory (DFT) calculation showed the cooperative water activation on lanthanide and O-O bond formation on transition metal for water oxidation. This work not only prepares a synthetic model of a bio-inspired oxygen-evolving center but also provides an effective strategy to realize light-driven overall water splitting.

引用

页数：9

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