An efficient catalytic hydrogenation of nitroarenes into their derived anilines is of critical importance for fine chemical industry and environmental remediation.Herein,a Cu decorated hollow carbon nanosphere(Cu/h-CS...An efficient catalytic hydrogenation of nitroarenes into their derived anilines is of critical importance for fine chemical industry and environmental remediation.Herein,a Cu decorated hollow carbon nanosphere(Cu/h-CS)was demonstrated as a promising nanoreactor to achieve enhanced hydrogenation toward nitroarene reduction.The unique hollow configuration of h-CS provided sufficient binding sites for Cu anchoring on interior and exterior surfaces,effectively preventing Cu agglomeration.The resulting homogenously dispersed Cu nanoparticles on h-CS exhibited a strong electronic interaction at the interface,leading to the generation of favorable electrophilic Cu^(δ+)sites.Meanwhile,thin shells with nanoporous channels enabled rapid electron migration,and regulated the mass transfer to boost reactant enrichment due to the void-confinement effect.Compared with its counterpart of Cu loaded solid carbon nanosphere(Cu/s-CS),the desirable structural and electronic configurations of Cu/h-CS offered a preferable micro-environment to achieve markedly enhanced catalytic activity in hydrogenation reactions.As an exemplary verification,the Cu/h-CS demonstrated a high turnover frequency of 740.74 h^(−1) for 4-nitrophenol reduction(~3-fold that of Cu/s-CS),an impressive reduction applicability toward a series of nitroarenes and azo-dyes,as well as an acceptable stability after 10 catalytic cycles.This work sheds new light on the design and construction of low-cost and high-performance catalysts for wide hydrogenation applications.展开更多
基金supported by the National Natural Science Foundation of China(Nos.22278228,32271789,and 52276200)the Ministry of Science and Technology of the People’s Republic of China(No.2018YFE0183600).
文摘An efficient catalytic hydrogenation of nitroarenes into their derived anilines is of critical importance for fine chemical industry and environmental remediation.Herein,a Cu decorated hollow carbon nanosphere(Cu/h-CS)was demonstrated as a promising nanoreactor to achieve enhanced hydrogenation toward nitroarene reduction.The unique hollow configuration of h-CS provided sufficient binding sites for Cu anchoring on interior and exterior surfaces,effectively preventing Cu agglomeration.The resulting homogenously dispersed Cu nanoparticles on h-CS exhibited a strong electronic interaction at the interface,leading to the generation of favorable electrophilic Cu^(δ+)sites.Meanwhile,thin shells with nanoporous channels enabled rapid electron migration,and regulated the mass transfer to boost reactant enrichment due to the void-confinement effect.Compared with its counterpart of Cu loaded solid carbon nanosphere(Cu/s-CS),the desirable structural and electronic configurations of Cu/h-CS offered a preferable micro-environment to achieve markedly enhanced catalytic activity in hydrogenation reactions.As an exemplary verification,the Cu/h-CS demonstrated a high turnover frequency of 740.74 h^(−1) for 4-nitrophenol reduction(~3-fold that of Cu/s-CS),an impressive reduction applicability toward a series of nitroarenes and azo-dyes,as well as an acceptable stability after 10 catalytic cycles.This work sheds new light on the design and construction of low-cost and high-performance catalysts for wide hydrogenation applications.
