TY - JOUR
T1 - Efficient charge separation by a donor-acceptor system integrating dibenzothiophene into a porphyrin-based metal-organic framework for enhanced photocatalytic hydrogen evolution
AU - Yan, Fei
AU - Zhang, Youzi
AU - Liu, Sibi
AU - Zou, Ruiqing
AU - Ghasemi, Jahan B.
AU - Li, Xuanhua
N1 - Publisher Copyright:
© 2023 Dalian Institute of Chemical Physics, the Chinese Academy of Sciences
PY - 2023/8
Y1 - 2023/8
N2 - The high selectivity of organic ligands and metal ions that construct metal-organic frameworks (MOFs) enables considerable richness in the MOF structure and confers them with numerous potentials, rendering MOFs extremely interesting to researchers in the field of photocatalytic hydrogen evolution. However, the severe recombination of photoinduced charge carriers significantly restricts the photocatalytic performance of the MOFs. Herein, we report a porphyrin-based donor-acceptor (D-A) MOF consisting of meso-tetra(4-carboxyphenyl) porphyrin (TCPP) donor and a thieno [3,2b:20,30-d]thiophene-S,S-dioxide (BTDO) acceptor via coordination with Zn2+ ions, and denoted as TCPP-Zn-BTDO. The charge-transfer interaction from TCPP to BTDO broadened the light absorption range of TCPP-Zn-BTDO, with a high theoretical spectral efficiency of 69.72%. The D-A structure of TCPP-Zn-BTDO effectively enhanced the internal electric field because of its large molecular dipole, which significantly improved the charge-separation efficiency. Based on the aforementioned improvements, TCPP-Zn-BTDO showed a three-fold higher photocatalytic hydrogen evolution rate than the corresponding monocomponent MOF of TCPP-Zn without the BTDO acceptor. The D-A MOF reported in this study provides a new strategy for enhancing the photocatalytic performance of MOF.
AB - The high selectivity of organic ligands and metal ions that construct metal-organic frameworks (MOFs) enables considerable richness in the MOF structure and confers them with numerous potentials, rendering MOFs extremely interesting to researchers in the field of photocatalytic hydrogen evolution. However, the severe recombination of photoinduced charge carriers significantly restricts the photocatalytic performance of the MOFs. Herein, we report a porphyrin-based donor-acceptor (D-A) MOF consisting of meso-tetra(4-carboxyphenyl) porphyrin (TCPP) donor and a thieno [3,2b:20,30-d]thiophene-S,S-dioxide (BTDO) acceptor via coordination with Zn2+ ions, and denoted as TCPP-Zn-BTDO. The charge-transfer interaction from TCPP to BTDO broadened the light absorption range of TCPP-Zn-BTDO, with a high theoretical spectral efficiency of 69.72%. The D-A structure of TCPP-Zn-BTDO effectively enhanced the internal electric field because of its large molecular dipole, which significantly improved the charge-separation efficiency. Based on the aforementioned improvements, TCPP-Zn-BTDO showed a three-fold higher photocatalytic hydrogen evolution rate than the corresponding monocomponent MOF of TCPP-Zn without the BTDO acceptor. The D-A MOF reported in this study provides a new strategy for enhancing the photocatalytic performance of MOF.
KW - Charge separation
KW - Donor-acceptor
KW - Metal-organic framework
KW - Photocatalysis
KW - Porphyrin
UR - http://www.scopus.com/inward/record.url?scp=85170696237&partnerID=8YFLogxK
U2 - 10.1016/S1872-2067(23)64475-4
DO - 10.1016/S1872-2067(23)64475-4
M3 - 文章
AN - SCOPUS:85170696237
SN - 1872-2067
VL - 51
SP - 124
EP - 134
JO - Chinese Journal of Catalysis
JF - Chinese Journal of Catalysis
ER -