TY - JOUR
T1 - A long-range synergistic effect between Ptn clusters and Zn1 single atoms for efficient selective hydrogenations
AU - Wei, Haisheng
AU - Li, Jing
AU - Yan, Xiaorui
AU - Liu, Tiantian
AU - Li, Kairui
AU - Feng, Dan
AU - Ren, Yujing
N1 - Publisher Copyright:
© 2024 The Royal Society of Chemistry.
PY - 2024/10/4
Y1 - 2024/10/4
N2 - Supported platinum group metal (PGM) catalysts are extensively utilized in catalytic hydrogenations. However, the adsorption energies on single PGM surfaces present the inherent scaling properties, which often lead to increased hydrogenation activity at the expense of selectivity. To address this challenge, we developed a space-separated strategy by confining few-atom Ptn clusters in Zn1-N3 sites decorated with microporous carbon material (Ptn@Zn1-N-C) to break the scaling relationship in selective hydrogenations. In detail, Ptn clusters are more favorable for H2 activation, while the Zn1-N3 single-atom sites can preferentially adsorb functional groups with electron-rich oxygen atoms. Benefiting from this long-range synergistic effect, the Ptn@Zn1-N-C catalyst displays superior catalytic performance in the selective hydrogenation of nitroarenes (>99% selectivity at ∼100% conversion, and sulfur compound-resistant hydrogenations) and excellent stability in the reverse water gas shift reaction (>99% selectivity over 40 hours at 600 °C). Our findings provide a confinement approach for further improving catalytic performance in selective hydrogenations.
AB - Supported platinum group metal (PGM) catalysts are extensively utilized in catalytic hydrogenations. However, the adsorption energies on single PGM surfaces present the inherent scaling properties, which often lead to increased hydrogenation activity at the expense of selectivity. To address this challenge, we developed a space-separated strategy by confining few-atom Ptn clusters in Zn1-N3 sites decorated with microporous carbon material (Ptn@Zn1-N-C) to break the scaling relationship in selective hydrogenations. In detail, Ptn clusters are more favorable for H2 activation, while the Zn1-N3 single-atom sites can preferentially adsorb functional groups with electron-rich oxygen atoms. Benefiting from this long-range synergistic effect, the Ptn@Zn1-N-C catalyst displays superior catalytic performance in the selective hydrogenation of nitroarenes (>99% selectivity at ∼100% conversion, and sulfur compound-resistant hydrogenations) and excellent stability in the reverse water gas shift reaction (>99% selectivity over 40 hours at 600 °C). Our findings provide a confinement approach for further improving catalytic performance in selective hydrogenations.
UR - http://www.scopus.com/inward/record.url?scp=85206493789&partnerID=8YFLogxK
U2 - 10.1039/d4qi02027h
DO - 10.1039/d4qi02027h
M3 - 文章
AN - SCOPUS:85206493789
SN - 2052-1553
VL - 11
SP - 7822
EP - 7830
JO - Inorganic Chemistry Frontiers
JF - Inorganic Chemistry Frontiers
IS - 22
ER -