Reordering d Orbital Energies of Single‐Site Catalysts for CO2 Electroreduction
Author(s)
Han, Jianyu
An, Pengfei
Liu, Shuhu
Zhang, Xiaofei
Wang, Dawei
Yuan, Yi
Guo, Jun
Qiu, Xueying
Hou, Ke
Shi, Lin
Zhang, Yin
Zhao, Shenlong
Long, Chang
Tang, Zhiyong
Griffith University Author(s)
Year published
2019
Metadata
Show full item recordAbstract
The single‐site catalyst (SSC) characteristic of atomically dispersed active centers will not only maximize the catalytic activity, but also provide a promising platform for establishing the structure–activity relationship. However, arbitrary arrangements of active sites in the existed SSCs make it difficult for mechanism understanding and performance optimization. Now, a well‐defined ultrathin SSC is fabricated by assembly of metal‐porphyrin molecules, which enables the precise identification of the active sites for d‐orbital energy engineering. The activity of as‐assembled products for electrocatalytic CO2 reduction is ...
View more >The single‐site catalyst (SSC) characteristic of atomically dispersed active centers will not only maximize the catalytic activity, but also provide a promising platform for establishing the structure–activity relationship. However, arbitrary arrangements of active sites in the existed SSCs make it difficult for mechanism understanding and performance optimization. Now, a well‐defined ultrathin SSC is fabricated by assembly of metal‐porphyrin molecules, which enables the precise identification of the active sites for d‐orbital energy engineering. The activity of as‐assembled products for electrocatalytic CO2 reduction is significantly promoted via lifting up the energy level of metal durn:x-wiley:14337851:media:anie201907399:anie201907399-math-0001 orbitals, exhibiting a remarkable Faradaic efficiency of 96 % at the overpotential of 500 mV. Furthermore, a turnover frequency of 4.21 s−1 is achieved with negligible decay over 48 h.
View less >
View more >The single‐site catalyst (SSC) characteristic of atomically dispersed active centers will not only maximize the catalytic activity, but also provide a promising platform for establishing the structure–activity relationship. However, arbitrary arrangements of active sites in the existed SSCs make it difficult for mechanism understanding and performance optimization. Now, a well‐defined ultrathin SSC is fabricated by assembly of metal‐porphyrin molecules, which enables the precise identification of the active sites for d‐orbital energy engineering. The activity of as‐assembled products for electrocatalytic CO2 reduction is significantly promoted via lifting up the energy level of metal durn:x-wiley:14337851:media:anie201907399:anie201907399-math-0001 orbitals, exhibiting a remarkable Faradaic efficiency of 96 % at the overpotential of 500 mV. Furthermore, a turnover frequency of 4.21 s−1 is achieved with negligible decay over 48 h.
View less >
Journal Title
Angewandte Chemie - International Edition
Volume
58
Issue
36
Subject
Chemical sciences
2D materials
CO2 reduction
electrocatalysis
orbital reordering
single-site catalysts