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High‐Density and Thermally Stable Palladium Single‐Atom Catalysts for Chemoselective Hydrogenations
Author(s) -
Ma Ying,
Ren Yujing,
Zhou Yanan,
Liu Wei,
Baaziz Walid,
Ersen Ovidiu,
PhamHuu Cuong,
Greiner Mark,
Chu Wei,
Wang Aiqin,
Zhang Tao,
Liu Yuefeng
Publication year - 2020
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202007707
Subject(s) - catalysis , selectivity , palladium , carbide , atom (system on chip) , oxide , vacancy defect , phase (matter) , materials science , density functional theory , photochemistry , atmosphere (unit) , chemistry , chemical engineering , crystallography , computational chemistry , organic chemistry , metallurgy , thermodynamics , physics , computer science , embedded system , engineering
Abstract Single‐atom catalysts (SACs) have shown superior activity and/or selectivity for many energy‐ and environment‐related reactions, but their stability at high site density and under reducing atmosphere remains unresolved. Herein, we elucidate the intrinsic driving force of a Pd single atom with high site density (up to 5 wt %) under reducing atmosphere, and its unique catalytic performance for hydrogenation reactions. In situ experiments and calculations reveal that Pd atoms tend to migrate into the surface vacancy‐enriched MoC surface during the carburization process by transferring oxide crystals to carbide crystals, leading to the surface enrichment of atomic Pd instead of formation of particles. The Pd 1 /α‐MoC catalyst exhibits high activity and excellent selectivity for liquid‐phase hydrogenation of substituted nitroaromatics (>99 %) and gas‐phase hydrogenation of CO 2 to CO (>98 %). The Pd 1 /α‐MoC catalyst could endure up to 400 °C without any observable aggregation of single atoms.