Metal oxides have been used as the supports for heterogeneous catalysis formany years,but they still suffer from coking in some high-temperature applications.The main reasons for coking are the uncontrollable dissocia...Metal oxides have been used as the supports for heterogeneous catalysis formany years,but they still suffer from coking in some high-temperature applications.The main reasons for coking are the uncontrollable dissociation of C-H and the overbalance between carbon deposition and removal.Herein,we find a boron nitride(BN)-immobilized Ni catalyst shows unprecedented coking resistance in dry reforming of methane via the incomplete decomposition of methane.Unlike the Ni-based catalysts supported by traditional metal oxides,BN-supported Ni accelerates the first C-H dissociation while inhibiting the breaking of the final C-H bond;hence,the suppression of the complete decomposition of methane thoroughly addresses the coking issue.This work reveals the fundamental reason for the coking resistance over BN-supported Ni catalysts is selective activation of the C-H bond,which can provide an inspiring idea for other applications.展开更多
Single-atom catalysts(SACs)are promising in some reactions typically promoted by homogeneous catalysts.However,the leaching of active species from the support in liquid-phase reactions hinders their potential applicat...Single-atom catalysts(SACs)are promising in some reactions typically promoted by homogeneous catalysts.However,the leaching of active species from the support in liquid-phase reactions hinders their potential applications.Herein,taking the hydroformylation reaction as an example,we report ionic liquid(IL)-induced stabilization of single Rh atoms against leaching.Among the ILs examined.展开更多
基金financial support from the National Natural Science Foundation of China(grant nos.22006098 and 22125604)Shanghai Sailing Program(grant no.20YF1413300)+1 种基金J.D.thanks Dr.Lei Xie at Fudan University for fruitful discussions.The computational part is also supported by the JSPS KAKENHI(grant no.JP20K05217)the supercomputer at RCCS(grant no.22-IMS-C002),Okazaki,Japan.
文摘Metal oxides have been used as the supports for heterogeneous catalysis formany years,but they still suffer from coking in some high-temperature applications.The main reasons for coking are the uncontrollable dissociation of C-H and the overbalance between carbon deposition and removal.Herein,we find a boron nitride(BN)-immobilized Ni catalyst shows unprecedented coking resistance in dry reforming of methane via the incomplete decomposition of methane.Unlike the Ni-based catalysts supported by traditional metal oxides,BN-supported Ni accelerates the first C-H dissociation while inhibiting the breaking of the final C-H bond;hence,the suppression of the complete decomposition of methane thoroughly addresses the coking issue.This work reveals the fundamental reason for the coking resistance over BN-supported Ni catalysts is selective activation of the C-H bond,which can provide an inspiring idea for other applications.
基金from the Singapore National Research Foundation(ANR-17-CE06-001701 and WBS:R-279-000-530-281)for their finiancial support.The XAS were collected at the beamline BL01B1 at the SPring-8(Japan Synchrotron Radiation Research Institute,Hyogo,Japan)under the approval of JASRI(Proposal No.2019A1398).Q.H.thanks the NRF Fellowship(NRF-NRFF11-2019-0002)from the National Research Foundation of Singapore.M.G.and J.H.acknowledge the MEXT Project of Integrated Research Consortium on Chemical Science(IRCCS),the Photoexcitonix Project at Hokkaido University,and JSPS KAKENHI(JP20K05217).Some of the computations were performed at RCCS(Okazaki,Japan).
文摘Single-atom catalysts(SACs)are promising in some reactions typically promoted by homogeneous catalysts.However,the leaching of active species from the support in liquid-phase reactions hinders their potential applications.Herein,taking the hydroformylation reaction as an example,we report ionic liquid(IL)-induced stabilization of single Rh atoms against leaching.Among the ILs examined.
