Indium oxide(In_(2)O_(3)),as a promising candidate for CO_(2)hydrogenation to C_(1) products,often suffers from sintering and activity decline,closely related to the undesirable structural evolution under reaction con...Indium oxide(In_(2)O_(3)),as a promising candidate for CO_(2)hydrogenation to C_(1) products,often suffers from sintering and activity decline,closely related to the undesirable structural evolution under reaction conditions.Based on the comprehension of the dynamic evolution,this study presents an efficient strategy to alleviate the agglomeration of In_(2)O_(3)nanoparticles by the surface decoration with highly dispersed silica species(SiO_(x)).Various structural characterizations combined with density functional theory calculations demonstrated that the sintering resulted from the over-reduction,while the enhanced stability originated from the anchoring effect of highly stable In-OSi bonds,which hinders the substantial formation of metallic In(In^(0))and the subsequent agglomeration.0.6Si/In_(2)O_(3)exhibited CO_(2)conversion rate of10.0 mmol g^(-1)h^(-1)at steady state vs.3.5 mmol g^(-1)h^(-1)on In_(2)O_(3)in CO_(2)hydrogenation.Enhanced steady-state activity was also achieved on Pd-modified catalysts.Compared to the traditional Pd/In_(2)O_(3)catalyst,the methanol production rate of Pd catalyst supported on 0.6Si/In_(2)O_(3)was enhanced by 23%,showing the potential of In_(2)O_(3)modified by SiO_(x)in serving as a platform material.This work provides a promising method to design new In_(2)O_(3)-based catalysts with improved activity and stability in CO_(2)hydrogenation.展开更多
We report that oxygen vacancies have a profound impact on phase separation and thermoelectric properties of ITO films grown at room temperature.Oxygen vacancies in non-stoichiometric In1.8Sn0.2O2.5 films aided the for...We report that oxygen vacancies have a profound impact on phase separation and thermoelectric properties of ITO films grown at room temperature.Oxygen vacancies in non-stoichiometric In1.8Sn0.2O2.5 films aided the formation of In-rich metallic clusters.It yields a high electrical conductivity s=1540 Scm1 and Seebeck coefficient|a|=27.2 mVK1,which resulted in the highest power factor(a2 s=113.8 mW m1 K2)but low optical transmission(Top-25%).An increase in oxygen partial pressure resulted in stochiometric In1.8Sn0.2O3 films which improved the optical transparency by 300%(Top-75.4%),but power factor was reduced by-85%due to a decrease in a and s.A decrease in a was due to the lack of energy filtering of charge carriers in the stoichiometric ITO film which did not have In-rich metallic clusters.XPS results showed that the valence band energy shifts with a change in oxygen partial pressure due to a decrease in carrier density,which implied a change in Fermi energy due to the reverse Moss-Burstein effect.Our results showed that phase separation can be obtained in nanocomposite ITO films by tuning their stoichiometry simply by varying the oxygen partial pressure during deposition of thermoelectric materials at low temperatures.展开更多
Controlling fluid flow in capillaric circuits is a key requirement to increase their uptake for assay applications.Capillary action off-valves provide such functionality by pushing an occluding bubble into the channel...Controlling fluid flow in capillaric circuits is a key requirement to increase their uptake for assay applications.Capillary action off-valves provide such functionality by pushing an occluding bubble into the channel using a difference in capillary pressure.Previously,we utilized the binary switching mode of this structure to develop a powerful set of fundamental fluidic valving operations.In this work,we study the transistor-like qualities of the off-valve and provide evidence that these structures are in fact functionally complementary to electronic junction field effect transistors.In view of this,we propose the new term capillaric field effect transistor to describe these types of valves.To support this conclusion,we present a theoretical description,experimental characterization,and practical application of analog flow resistance control.In addition,we demonstrate that the valves can also be reopened.We show modulation of the flow resistance from fully open to pinch-off,determine the flow rate-trigger channel volume relationship and demonstrate that the latter can be modeled using Shockley's equation for electronic transistors.Finally,we provide a first example of how the valves can be opened and closed repeatedly.展开更多
基金financially supported by the National Natural Science Foundation of China(22172013)the Special Project for Key Research and Development Program of Xinjiang Autonomous Region(2022B01033-3)+3 种基金the Liaoning Revitalization Talent Program(XLYC2008032 and XLYC2203126)the Fundamental Research Funds for the Central Universities(DUT22LK24,DUT22QN207 and DUT22LAB602)the CUHK Research Startup Fund(No.#4930981)financial support from Catalyst:Seeding funding(CSG-VUW2201)provided by the New Zealand Ministry of Business,Innovation and Employment and administered by the Royal Society Aparangi。
文摘Indium oxide(In_(2)O_(3)),as a promising candidate for CO_(2)hydrogenation to C_(1) products,often suffers from sintering and activity decline,closely related to the undesirable structural evolution under reaction conditions.Based on the comprehension of the dynamic evolution,this study presents an efficient strategy to alleviate the agglomeration of In_(2)O_(3)nanoparticles by the surface decoration with highly dispersed silica species(SiO_(x)).Various structural characterizations combined with density functional theory calculations demonstrated that the sintering resulted from the over-reduction,while the enhanced stability originated from the anchoring effect of highly stable In-OSi bonds,which hinders the substantial formation of metallic In(In^(0))and the subsequent agglomeration.0.6Si/In_(2)O_(3)exhibited CO_(2)conversion rate of10.0 mmol g^(-1)h^(-1)at steady state vs.3.5 mmol g^(-1)h^(-1)on In_(2)O_(3)in CO_(2)hydrogenation.Enhanced steady-state activity was also achieved on Pd-modified catalysts.Compared to the traditional Pd/In_(2)O_(3)catalyst,the methanol production rate of Pd catalyst supported on 0.6Si/In_(2)O_(3)was enhanced by 23%,showing the potential of In_(2)O_(3)modified by SiO_(x)in serving as a platform material.This work provides a promising method to design new In_(2)O_(3)-based catalysts with improved activity and stability in CO_(2)hydrogenation.
基金the Ministry of Business,Innovation and Employment(MBIE),New Zealand(contract#C05X1802).TM acknowledges support from JST Mirai Program JPMJMI19A1.
文摘We report that oxygen vacancies have a profound impact on phase separation and thermoelectric properties of ITO films grown at room temperature.Oxygen vacancies in non-stoichiometric In1.8Sn0.2O2.5 films aided the formation of In-rich metallic clusters.It yields a high electrical conductivity s=1540 Scm1 and Seebeck coefficient|a|=27.2 mVK1,which resulted in the highest power factor(a2 s=113.8 mW m1 K2)but low optical transmission(Top-25%).An increase in oxygen partial pressure resulted in stochiometric In1.8Sn0.2O3 films which improved the optical transparency by 300%(Top-75.4%),but power factor was reduced by-85%due to a decrease in a and s.A decrease in a was due to the lack of energy filtering of charge carriers in the stoichiometric ITO film which did not have In-rich metallic clusters.XPS results showed that the valence band energy shifts with a change in oxygen partial pressure due to a decrease in carrier density,which implied a change in Fermi energy due to the reverse Moss-Burstein effect.Our results showed that phase separation can be obtained in nanocomposite ITO films by tuning their stoichiometry simply by varying the oxygen partial pressure during deposition of thermoelectric materials at low temperatures.
基金The authors would like to thank Helen Devereux and Gary Turner of the Nanofabrication Laboratory at the University of Canterbury for technical support.Funding was provided by MBIE Grant UOCX1706.CM.acknowledges support in form of a JSPS Postdoctoral Fellowship for Research in Japan.V.N.acknowledges Rutherford Discovery Fellowship RDF-19-UOC-019for additional funding.
文摘Controlling fluid flow in capillaric circuits is a key requirement to increase their uptake for assay applications.Capillary action off-valves provide such functionality by pushing an occluding bubble into the channel using a difference in capillary pressure.Previously,we utilized the binary switching mode of this structure to develop a powerful set of fundamental fluidic valving operations.In this work,we study the transistor-like qualities of the off-valve and provide evidence that these structures are in fact functionally complementary to electronic junction field effect transistors.In view of this,we propose the new term capillaric field effect transistor to describe these types of valves.To support this conclusion,we present a theoretical description,experimental characterization,and practical application of analog flow resistance control.In addition,we demonstrate that the valves can also be reopened.We show modulation of the flow resistance from fully open to pinch-off,determine the flow rate-trigger channel volume relationship and demonstrate that the latter can be modeled using Shockley's equation for electronic transistors.Finally,we provide a first example of how the valves can be opened and closed repeatedly.