Unveiling the pore-size performance of metal organic frameworks(MOFs)is imperative for controllable design of sophisticated catalysts.Herein,UiO-66 with distinct macropores and mesopores were intentionally created and...Unveiling the pore-size performance of metal organic frameworks(MOFs)is imperative for controllable design of sophisticated catalysts.Herein,UiO-66 with distinct macropores and mesopores were intentionally created and served as substrates to create advanced CdS/UiO-66 catalysts.The pore size impacted the spatial distribution of CdS nanoparticles(NPs):CdS tended to deposit on the external surface of mesoporous UiO-66,but spontaneously penetrated into the large cavity of macroporous UiO-66 nanocage.Normalized to unit amount of CdS,the photocatalytic reaction constant of macroporous CdS/UiO-66 over 4-nitroaniline reduction was~3 folds of that of mesoporous counterpart,and outperformed many other reported state-of-art CdS-based catalysts.A confinement effect of CdS NPs within UiO-66 cage could respond for its high activity,which could shorten the electron-transport distance of NPs-MOFs-reactant,and protect the active CdS NPs from photocorrosion.The finding here provides a straightforward paradigm and mechanism to rationally fabricate advance NPs/MOFs for diverse applications.展开更多
MoS2 is a promising candidate for catalyzing hydrogen evolution reaction (HER) due to its low cost and high activity. However, the poor conductivity and the stack of active sites of bulk MoS2 hinder its application. H...MoS2 is a promising candidate for catalyzing hydrogen evolution reaction (HER) due to its low cost and high activity. However, the poor conductivity and the stack of active sites of bulk MoS2 hinder its application. Herein, a new facile solid-state synthesis strategy was developed to fabricate MoS2 nanorods by one-step pyrolysis of molybdenum-organic framework (Mo-MOF) in the presence of thiourea. The obtained MoS2 keeps the Mo-MOF nanorod structure with more active sites, while the residual carbon left in the nanorod enhances the conductivity. The as-prepared MoS2 nanorods exhibit superior stability and excellent activity towards HER with a small onset potential of 96 mV and a low Tafel slope of 93 mV decade^-1.展开更多
基金the National Natural Science Foundation of China(22022412,21874155,22104060)the Natural Science Foundation of Jiangsu Province(BK20200716,BK20191316)+3 种基金the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(20KJB150019)Innovation and Entrepreneurship Doctor Program of Jiangsu Province(JSSCBS20210317)the State Key Laboratory of Analytical Chemistry for Life Science(SKLACLS2106)the Qing-Lan Project of Jiangsu Province(2019)。
文摘Unveiling the pore-size performance of metal organic frameworks(MOFs)is imperative for controllable design of sophisticated catalysts.Herein,UiO-66 with distinct macropores and mesopores were intentionally created and served as substrates to create advanced CdS/UiO-66 catalysts.The pore size impacted the spatial distribution of CdS nanoparticles(NPs):CdS tended to deposit on the external surface of mesoporous UiO-66,but spontaneously penetrated into the large cavity of macroporous UiO-66 nanocage.Normalized to unit amount of CdS,the photocatalytic reaction constant of macroporous CdS/UiO-66 over 4-nitroaniline reduction was~3 folds of that of mesoporous counterpart,and outperformed many other reported state-of-art CdS-based catalysts.A confinement effect of CdS NPs within UiO-66 cage could respond for its high activity,which could shorten the electron-transport distance of NPs-MOFs-reactant,and protect the active CdS NPs from photocorrosion.The finding here provides a straightforward paradigm and mechanism to rationally fabricate advance NPs/MOFs for diverse applications.
基金the financial support from the National Key Research and Development Program of China (2017YFA0700100 and 2018YFA0208600)Strategic Priority Research Program of the Chinese Academy of Sciences (XDB20000000)+2 种基金National Natural Science Foundation of China (21671188, 21871263 and 21331006)Key Research Program of Frontier Science, CAS (QYZDJSSW-SLH045)Youth Innovation Promotion Association, CAS (2014265)
文摘MoS2 is a promising candidate for catalyzing hydrogen evolution reaction (HER) due to its low cost and high activity. However, the poor conductivity and the stack of active sites of bulk MoS2 hinder its application. Herein, a new facile solid-state synthesis strategy was developed to fabricate MoS2 nanorods by one-step pyrolysis of molybdenum-organic framework (Mo-MOF) in the presence of thiourea. The obtained MoS2 keeps the Mo-MOF nanorod structure with more active sites, while the residual carbon left in the nanorod enhances the conductivity. The as-prepared MoS2 nanorods exhibit superior stability and excellent activity towards HER with a small onset potential of 96 mV and a low Tafel slope of 93 mV decade^-1.
