Mesocrystals, the non-classical crystals with highly ordered nanoparticle superstructures, have shown great potential in many applications because of their newly collective properties. However, there is still a lack o...Mesocrystals, the non-classical crystals with highly ordered nanoparticle superstructures, have shown great potential in many applications because of their newly collective properties. However, there is still a lack of a facile and general synthesis strategy to organize and integrate distinct components into complex mesocrystals, and of reported application for them in industrial catalytic reactions. Herein we report a general bottom-up synthesis of CuO-based trimetallic oxide mesocrystals (denoted as CuO-M1Ox-M2Oy, where M1 and M2 = Zn, In, Fe, Ni, Mn, and Co) using a simple precipitation method followed by a hydrothermal treatment and a topotactic transformation via calcination. When these mesocrystals were used as the catalyst to produce trichlorosilane (TCS) via Si hydrochlorination reaction, they exhibited excellent catalytic performance with much increased Si conversion and TCS selectivity. In particular, the TCS yield was increased 19-fold than that of the catalyst-free process. The latter is the current industrial process. The efficiently catalytic property of these mesocrystals is attributed to the formation of well-defined nanoscale heterointerfaces that can effectively facilitate the charge transfer, and the generation of the compressive and tensile strain on CuO near the interfaces among different metal oxides. The synthetic approach developed here could be applicable to fabricate versatile complicated metal oxide mesocrystals as novel catalysts for various industrial chemical reactions.展开更多
Mercury emission has become a great environmental concern because of its high toxicity,bioaccumulation,and persistence.Adsorption is an effective method to remove Hg^(0)from coal-fired flue gas,with adsorbents playing...Mercury emission has become a great environmental concern because of its high toxicity,bioaccumulation,and persistence.Adsorption is an effective method to remove Hg^(0)from coal-fired flue gas,with adsorbents playing a dominant role.Extensive investigations have been conducted on the use of CuO-based materials for Hg^(0)removal,and some fruitful results have been obtained.In this review,we summarize advances in the application of CuO-based materials for Hg^(0)capture.Firstly,the fundamentals of CuO,including its crystal information and synthesis methods,are introduced.Then,the Hg^(0)removal capability of some typical CuO-based adsorbents is discussed.Considering that coal-fired flue gas also contains a certain amount of NO,SO_(2),H_(2)O,NH_(3),and HCl,the impacts of these species on adsorbent Hg^(0)removal efficiency are summarized next.By generalizing the mechanisms dominating the Hg^(0)removal process,the rate-determining step and the key intermediates can be discovered.Apart from Hg^(0),some other air pollutants,such as CO,NOx,and volatile organic compounds(VOCs),account for a certain portion of flue gas.In view of their similar abatement mechanisms,simultaneous removal of Hg^(0)and other air pollutants has become a hot topic in the environmental field.Considering the Hg^(0)re-emission phenomena in wet flue gas desulfurization(WFGD),mercury capture performance under different conditions in this device is discussed.Finally,we conclude that new adsorbents suitable for long-term operation in coal-fired flue gas should be developed to realize the effective reduction of mercury emissions.展开更多
基金the National Natural Science Foundation of China(Nos.21878301,21978299,and 21908224)Z.Z.thanks the kind support of Guangdong Technion Israel Institute of Technology(GTTIT)for the collaboration.
文摘Mesocrystals, the non-classical crystals with highly ordered nanoparticle superstructures, have shown great potential in many applications because of their newly collective properties. However, there is still a lack of a facile and general synthesis strategy to organize and integrate distinct components into complex mesocrystals, and of reported application for them in industrial catalytic reactions. Herein we report a general bottom-up synthesis of CuO-based trimetallic oxide mesocrystals (denoted as CuO-M1Ox-M2Oy, where M1 and M2 = Zn, In, Fe, Ni, Mn, and Co) using a simple precipitation method followed by a hydrothermal treatment and a topotactic transformation via calcination. When these mesocrystals were used as the catalyst to produce trichlorosilane (TCS) via Si hydrochlorination reaction, they exhibited excellent catalytic performance with much increased Si conversion and TCS selectivity. In particular, the TCS yield was increased 19-fold than that of the catalyst-free process. The latter is the current industrial process. The efficiently catalytic property of these mesocrystals is attributed to the formation of well-defined nanoscale heterointerfaces that can effectively facilitate the charge transfer, and the generation of the compressive and tensile strain on CuO near the interfaces among different metal oxides. The synthetic approach developed here could be applicable to fabricate versatile complicated metal oxide mesocrystals as novel catalysts for various industrial chemical reactions.
基金This work is supported by the Scientific Research Foundation of China Jiliang Universitythe Zhejiang Provincial Natural Science Foundation of China(Nos.LQ22E060003 and LY22E040001).
文摘Mercury emission has become a great environmental concern because of its high toxicity,bioaccumulation,and persistence.Adsorption is an effective method to remove Hg^(0)from coal-fired flue gas,with adsorbents playing a dominant role.Extensive investigations have been conducted on the use of CuO-based materials for Hg^(0)removal,and some fruitful results have been obtained.In this review,we summarize advances in the application of CuO-based materials for Hg^(0)capture.Firstly,the fundamentals of CuO,including its crystal information and synthesis methods,are introduced.Then,the Hg^(0)removal capability of some typical CuO-based adsorbents is discussed.Considering that coal-fired flue gas also contains a certain amount of NO,SO_(2),H_(2)O,NH_(3),and HCl,the impacts of these species on adsorbent Hg^(0)removal efficiency are summarized next.By generalizing the mechanisms dominating the Hg^(0)removal process,the rate-determining step and the key intermediates can be discovered.Apart from Hg^(0),some other air pollutants,such as CO,NOx,and volatile organic compounds(VOCs),account for a certain portion of flue gas.In view of their similar abatement mechanisms,simultaneous removal of Hg^(0)and other air pollutants has become a hot topic in the environmental field.Considering the Hg^(0)re-emission phenomena in wet flue gas desulfurization(WFGD),mercury capture performance under different conditions in this device is discussed.Finally,we conclude that new adsorbents suitable for long-term operation in coal-fired flue gas should be developed to realize the effective reduction of mercury emissions.