TY - JOUR
T1 - Stepping Out of Transition Metals: Activating the Dual Atomic Catalyst through Main Group Elements
AU - Sun, Mingzi
AU - Wong, Hon Ho
AU - Wu, Tong
AU - Dougherty, Alan William
AU - Huang, Bolong
N1 - Funding Information:
The authors gratefully acknowledge the support of the Natural Science Foundation of China (Grant No.: NSFC 21771156), and the Early Career Scheme (ECS) fund (Grant no.: PolyU 253026/16P) from the Research Grant Council (RGC) in Hong Kong.
Publisher Copyright:
© 2021 Wiley-VCH GmbH
PY - 2021/8/12
Y1 - 2021/8/12
N2 - In recent years, investigations into atomic catalysts has accelerated significantly. Although different atomic catalysts have been developed, the introduction of main group elements is rarely considered. In this work, the possibility of introducing alkaline/alkaline earth metals (AAEM), post-transition metal (Post-TM), and metalloids to form stable graphdiyne-based dual atomic catalysts (GDY-DAC) is revealed. The main group elements not only act as a promising separator to improve the loading of DACs but also activate the alkyl chains to facilitate the electroactivity of GDY-DAC. Most importantly, the main group elements in the GDY-DAC do not affect the electroactivity of transition or lanthanide metals and even enable subtle modulations on the electronic structures. The p band center is a significant descriptor to modulate the electroactivity in oxides while their applications in the atomic catalysts are unclear. With the further evaluations of machine learning, it is found that the involvements of s-orbitals and p-orbitals perturb the prediction accuracies of both formation energies and p-band center, especially for the AAEM. This work supplies insights that are expected to aid progress in designing main group elements-based atomic catalysts, which opens a new avenue in designing advanced electrocatalysts.
AB - In recent years, investigations into atomic catalysts has accelerated significantly. Although different atomic catalysts have been developed, the introduction of main group elements is rarely considered. In this work, the possibility of introducing alkaline/alkaline earth metals (AAEM), post-transition metal (Post-TM), and metalloids to form stable graphdiyne-based dual atomic catalysts (GDY-DAC) is revealed. The main group elements not only act as a promising separator to improve the loading of DACs but also activate the alkyl chains to facilitate the electroactivity of GDY-DAC. Most importantly, the main group elements in the GDY-DAC do not affect the electroactivity of transition or lanthanide metals and even enable subtle modulations on the electronic structures. The p band center is a significant descriptor to modulate the electroactivity in oxides while their applications in the atomic catalysts are unclear. With the further evaluations of machine learning, it is found that the involvements of s-orbitals and p-orbitals perturb the prediction accuracies of both formation energies and p-band center, especially for the AAEM. This work supplies insights that are expected to aid progress in designing main group elements-based atomic catalysts, which opens a new avenue in designing advanced electrocatalysts.
KW - dual atomic catalysts
KW - graphdiyne
KW - machine-learning
KW - main group elements
KW - s–p–d couplings
UR - http://www.scopus.com/inward/record.url?scp=85108336396&partnerID=8YFLogxK
U2 - 10.1002/aenm.202101404
DO - 10.1002/aenm.202101404
M3 - Journal article
AN - SCOPUS:85108336396
SN - 1614-6832
VL - 11
JO - Advanced Energy Materials
JF - Advanced Energy Materials
IS - 30
M1 - 2101404
ER -