TY - JOUR
T1 - Tuning the electronic structure of bimetallic CoCu clusters for efficient hydrolysis of ammonia borane
AU - Chen, Yufeng
AU - Wang, Kang
AU - Nie, Kaiqi
AU - Wang, Jiaou
AU - Wang, Shifeng
AU - Feng, Kun
AU - Zhong, Jun
N1 - Funding Information:
We acknowledge the support from NSRL (MCD-A and MCD-B, Soochow Beamline for Energy Materials), BSRF (4B9B), and SSRF (11B) for the XAS experiments. This work is supported by the National Key R&D Program of China (2020YFA0406103), the National Natural Science Foundation of China ( U1932211 ), the Collaborative Innovation Center of Suzhou Nano Science & Technology, the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD), and the 111 Project.
Publisher Copyright:
© 2022 Elsevier B.V.
PY - 2023/1/1
Y1 - 2023/1/1
N2 - Efficient and low cost catalysts for the hydrogen production from ammonia borane (AB) are highly required to build up the upcoming hydrogen economy. Here we demonstrated that the non-active material could be directly transformed to highly active catalyst for the hydrolysis of AB when the surface parts were stripped to form tiny clusters on graphene oxide (GO), with the presence of strong cluster-support interaction. Moreover, the catalytic activity can be greatly enhanced by further tuning the electronic structure of clusters with various compositions. As a result, the final bimetallic CoCu catalyst on GO can achieve a high total turnover frequency (TOF) value of 72.4 (H2) mol/(Cat-metal) mol·min with an activation energy of 47.8 kJ/mol, which is over 3 times higher than the monometallic clusters on GO. The cluster-support interaction has been clearly identified by synchrotron radiation X-ray absorption spectroscopy. An internal charge transfer from Cu to Co in the clusters can also be identified, which will weaken the B-N bond in AB and then effectively accelerate the hydrolysis of AB to achieve the high performance.
AB - Efficient and low cost catalysts for the hydrogen production from ammonia borane (AB) are highly required to build up the upcoming hydrogen economy. Here we demonstrated that the non-active material could be directly transformed to highly active catalyst for the hydrolysis of AB when the surface parts were stripped to form tiny clusters on graphene oxide (GO), with the presence of strong cluster-support interaction. Moreover, the catalytic activity can be greatly enhanced by further tuning the electronic structure of clusters with various compositions. As a result, the final bimetallic CoCu catalyst on GO can achieve a high total turnover frequency (TOF) value of 72.4 (H2) mol/(Cat-metal) mol·min with an activation energy of 47.8 kJ/mol, which is over 3 times higher than the monometallic clusters on GO. The cluster-support interaction has been clearly identified by synchrotron radiation X-ray absorption spectroscopy. An internal charge transfer from Cu to Co in the clusters can also be identified, which will weaken the B-N bond in AB and then effectively accelerate the hydrolysis of AB to achieve the high performance.
KW - Ammonia borane
KW - Clusters
KW - Hydrolysis
KW - X-ray absorption spectroscopy
UR - http://www.scopus.com/inward/record.url?scp=85137289424&partnerID=8YFLogxK
U2 - 10.1016/j.cej.2022.138931
DO - 10.1016/j.cej.2022.138931
M3 - Article
AN - SCOPUS:85137289424
SN - 1385-8947
VL - 451
JO - Chemical Engineering Journal
JF - Chemical Engineering Journal
M1 - 138931
ER -