Selectivity-control has long been a central pursuit in organic chemistry.Most recent advances have focused on achieving individual forms of selectivity,such as chemo-,regio-,E/Z-,diastereo-,or enantioselectivity.Tradi...Selectivity-control has long been a central pursuit in organic chemistry.Most recent advances have focused on achieving individual forms of selectivity,such as chemo-,regio-,E/Z-,diastereo-,or enantioselectivity.Traditionally,multi-selectivities have been realized through one-dimensional linear synthetic routes,in which distinct sites are modified sequentially across multiple reaction steps.展开更多
Owing to unique advantages of patternability and high substrate compatibility,screen-printing allows for the fabrication of flexible perovskite solar cells(f-PSCs)with designable device patterns,while the defective an...Owing to unique advantages of patternability and high substrate compatibility,screen-printing allows for the fabrication of flexible perovskite solar cells(f-PSCs)with designable device patterns,while the defective and fragile contact at the buried interface seriously restricted the device performance.Herein,a series of siloxane coupling agents(SCAs)with different ending groups i.e.,-SH,-NH_(2),and-CN were incorporated at the SnO_(2)/perovskite interface,which can selectively interact with MA+and Pb^(2+)via hydrogen and coordination bonding,respectively.It was revealed that the selection of(3-Cyanopropyl)Triethoxysilane(CN-PTES)can regulate perovskite crystallization with accelerated nucleation and retarded crystal growth,leading to improved crystallinity with released residual lattice strain.Moreover,the incorporated CN-PTES aligned the energy structure of the underlying SnO_(2)and boosted the interfacial adhesion between perovskite and SnO_(2),resulting in facilitated electron extraction and enhanced interfacial fracture energy.Consequently,the first screen-printed f-PSCs with improved mechanical resistance were finally obtained.展开更多
Photocatalytic CH_(4) coupling into high-valued C_(2)H_(6) is highly attractive,whereas the photosynthetic rate,especially under oxygen-free system,is still unsatisfying.Here,we designed the negatively charged metal s...Photocatalytic CH_(4) coupling into high-valued C_(2)H_(6) is highly attractive,whereas the photosynthetic rate,especially under oxygen-free system,is still unsatisfying.Here,we designed the negatively charged metal supported on metal oxide nanosheets to activate the inert C-H bond in CH_(4)and hence accelerate CH_(4) coupling performance.As an example,the synthetic Au/ZnO porous nanosheets exhibit the C_(2)H_(6) photosynthetic rate of 1,121.6μmol g^(-1)_(cat)h^(-1)and the CH_(4) conversion rate of 2,374.6μmol g^(-1)_(cat)h^(-1) under oxygen-free system,2 orders of magnitude higher than those of previously reported photocatalysts.By virtue of several in situ spectroscopic techniques,it is established that the generated Au^(δ-)and O^-species together polarized the C-H bond,while the Au^(δ-)and O^-species jointly stabilized the CH_(3) intermediates,which favored the coupling of CH_(3) intermediate to photosynthesize C_(2)H_(6) instead of overoxidation into CO_(x).Thus,the design of dual active species is beneficial for achieving high-efficient CH_(4)-to-C_(2)H_(6) photoconversion.展开更多
文摘Selectivity-control has long been a central pursuit in organic chemistry.Most recent advances have focused on achieving individual forms of selectivity,such as chemo-,regio-,E/Z-,diastereo-,or enantioselectivity.Traditionally,multi-selectivities have been realized through one-dimensional linear synthetic routes,in which distinct sites are modified sequentially across multiple reaction steps.
基金supported by the Natural Science Foundation of China(22425903,U24A20568,61705102,62288102,22409091,22409090 and 62205142)the National Key R&D Program of China(2023YFB4204500,2020YFA07099003)+1 种基金the Jiangsu Provincial Departments of Science and Technology(BK20241875,BE2022023,BK20220010,and BZ2023060)the Excellent Doctoral Dissertation Cultivation Program of Nanjing Tech University(2023-02).
文摘Owing to unique advantages of patternability and high substrate compatibility,screen-printing allows for the fabrication of flexible perovskite solar cells(f-PSCs)with designable device patterns,while the defective and fragile contact at the buried interface seriously restricted the device performance.Herein,a series of siloxane coupling agents(SCAs)with different ending groups i.e.,-SH,-NH_(2),and-CN were incorporated at the SnO_(2)/perovskite interface,which can selectively interact with MA+and Pb^(2+)via hydrogen and coordination bonding,respectively.It was revealed that the selection of(3-Cyanopropyl)Triethoxysilane(CN-PTES)can regulate perovskite crystallization with accelerated nucleation and retarded crystal growth,leading to improved crystallinity with released residual lattice strain.Moreover,the incorporated CN-PTES aligned the energy structure of the underlying SnO_(2)and boosted the interfacial adhesion between perovskite and SnO_(2),resulting in facilitated electron extraction and enhanced interfacial fracture energy.Consequently,the first screen-printed f-PSCs with improved mechanical resistance were finally obtained.
基金supported by the National Key R&D Program of China(2019YFA0210004,2022YFA1502904,2021YFA1501502)the National Natural Science Foundation of China(22125503,21975242,U2032212,21890754,22002148)+1 种基金2023 Synchrotron Radiation Joint Fund of USTCthe Youth Innovation Promotion Association of CAS(CX2340007003)。
文摘Photocatalytic CH_(4) coupling into high-valued C_(2)H_(6) is highly attractive,whereas the photosynthetic rate,especially under oxygen-free system,is still unsatisfying.Here,we designed the negatively charged metal supported on metal oxide nanosheets to activate the inert C-H bond in CH_(4)and hence accelerate CH_(4) coupling performance.As an example,the synthetic Au/ZnO porous nanosheets exhibit the C_(2)H_(6) photosynthetic rate of 1,121.6μmol g^(-1)_(cat)h^(-1)and the CH_(4) conversion rate of 2,374.6μmol g^(-1)_(cat)h^(-1) under oxygen-free system,2 orders of magnitude higher than those of previously reported photocatalysts.By virtue of several in situ spectroscopic techniques,it is established that the generated Au^(δ-)and O^-species together polarized the C-H bond,while the Au^(δ-)and O^-species jointly stabilized the CH_(3) intermediates,which favored the coupling of CH_(3) intermediate to photosynthesize C_(2)H_(6) instead of overoxidation into CO_(x).Thus,the design of dual active species is beneficial for achieving high-efficient CH_(4)-to-C_(2)H_(6) photoconversion.
