Direct Z-scheme photochemical hybrid systems:Loading porphyrin-based metal-organic cages on graphitic-C_(3)N_(4) to dramatically enhance photocatalytic hydrogen evolution

作     者：Yang Lei Jian-Feng Huang Xin-Ao Li Chu-Ying Lv Chao-Ping Hou Jun-Min Liu 雷洋;黄剑锋;李鑫奥;吕楚滢;侯超苹;刘军民

作者机构：The Key Laboratory of Low-Carbon Chemistry&Energy Conservation of Guangdong ProvinceSchool of Materials Science and EngineeringSun Yat-sen UniversityGuangzhou 510275GuangdongChina 

基　　金：国家自然科学基金(21975291,21572280) 广东省自然科学基金(2019A1515011640,2022A1515011949,2020A1515110474,2018A030313479) 

出 版 物：《Chinese Journal of Catalysis》 (催化学报（英文）)

年 卷 期：2022年第43卷第8期

页      码：2249-2258页

摘      要：The rational design of photochemical molecular device(PMD)and its hybrid system has great potential in improving the activity of photocatalytic hydrogen production.A series of Pd6L3 type metal-organic cages,denoted as MOC-Py-M(M=H,Cu,and Zn),are designed for PMDs by combining metalloporphyrin-based ligands with catalytically active Pd^(2+)*** metal-organic cages(MOCs)are first successfully hybridized with graphitic carbon nitride(g-C_(3)N_(4))to form direct Z-scheme heterogeneous MOC-Py-M/g-C_(3)N_(4)(M=H,Cu,and Zn)photocatalysts via π-π*** from its better light absorption ability,the MOC-Py-Zn/g-C_(3)N_(4) catalyst exhibits high H_(2) production activity under visible light(10348μmol g^(-1) h^(-1)),far superior to MOC-Py-H/g-C_(3)N_(4) and MOC-Py-Cu/g-C_(3)N_(4).Moreover,the MOC-Py-Zn/g-C_(3)N_(4) system obtains an enhanced turn over number(TON)value of 32616 within 100 h,outperforming the homogenous MOC-Py-Zn(TON of 507 within 100 h),which is one of the highest photochemical hybrid systems based on MOC for visible-light-driven hydrogen *** confirms the direct Z-scheme heterostructure can promote effective charge transfer,expand the visible light absorption region,and protect the cages from decomposition in MOC-Py-Zn/g-C_(3)N_(4).This work presents a creative example that direct Z-scheme PMD-based systems for effective and persistent hydrogen generation from water under visible light are obtained by heterogenization approach using homogeneous porphyrin-based MOCs and g-C_(3)N_(4) semiconductors.

主 题 词：Porphyrin-based metal-organic cage g-C_(3)N_(4) Photochemical molecular device Direct Z-scheme heterostructure Photocatalytic hydrogen evolution from water 

学科分类：081702[081702] 081704[081704] 081705[081705] 07[理学] 0817[工学-轻工类] 08[工学] 070304[070304] 0703[理学-化学类] 

核心收录：

D　O　I：10.1016/S1872-2067(22)64109-3

馆 藏 号：203114067...