SnO_(2)electron transport layer(ETL)is a vital component in perovskite solar cells(PSCs),due to its excellent photoelectric properties and facile fabrication process.In this study,we synthesized a water-soluble and ad...SnO_(2)electron transport layer(ETL)is a vital component in perovskite solar cells(PSCs),due to its excellent photoelectric properties and facile fabrication process.In this study,we synthesized a water-soluble and adhesive polyelectrolyte with ethanolamine(EA)and poly-acrylic acid(PAA).The linear PAA was crosslinked by EA,forming a 3D network that stabilized the SnO_(2)nanoparticle dispersion.An organic–inorganic hybrid ETL is developed by introducing the cross-linked PAA-EA into SnO_(2)ETL,which prevents nano particle agglomeration and facilitates uniform SnO_(2)film formation with fewer defects.Additionally,the PAA-EA-modified SnO_(2)facilitated a uniform and compact perovskite film,enhancing the interface contact and carrier transport.Consequently,the PAA-EA-modified PSCs exhibited excellent PCE of 24.34%and 22.88%with high reproducibility for areas of 0.045 and 1.00 cm~2,respectively.Notably,owing to structure reinforce effect of PAA-EA in SnO_(2)ETL,flexible device demonstrated an impressive PCE of 23.34%while maintaining 90.1%of the initial PCE after 10,000 bending cycles with a bending radius of 5 mm.This successful approach of polyelectrolyte reinforced hybrid organic–inorganic ETL displays great potential for flexible,large-area PSCs application.展开更多
Thin film composite(TFC) membranes represent a highly promising platform for efficient nanofiltration(NF)processes. However, the improvement in permeance is impeded by the substrates with low permeances. Herein,highly...Thin film composite(TFC) membranes represent a highly promising platform for efficient nanofiltration(NF)processes. However, the improvement in permeance is impeded by the substrates with low permeances. Herein,highly permeable gradient phenolic membranes with tight selectivity are used as substrates to prepare TFC membranes with high permeances by the layer-by-layer assembly method. The negatively charged phenolic substrates are alternately assembled with polycation polyethylenimine(PEI) and polyanion poly(acrylic acid)(PAA)as a result of electrostatic interactions, forming thin and compact PEI/PAA layers tightly attached to the substrate surface. Benefiting from the high permeances and tight surface pores of the gradient nanoporous structures of the substrates, the produced PEI/PAA membranes exhibit a permeance up to 506 L? m-2?h-1?MPa-1, which is ~2–10 times higher than that of other membranes with similar rejections. The PEI/PAA membranes are capable of retaining N 96.1% of negatively charged dyes following the mechanism of electrostatic repulsion. We demonstrate that the membranes can also separate positively and neutrally charged dyes from water via other mechanisms.This work opens a new avenue for the design and preparation of high-flux NF membranes, which is also applicable to enhance the permeance of other TFC membranes.展开更多
The authors have investigated the pH and ionic strength response of self-assembled layers formed by adsorption of amphiphilic weak polyelectrolytes. Using the SFA （Surface Forces Apparatus） the authors measured forc...The authors have investigated the pH and ionic strength response of self-assembled layers formed by adsorption of amphiphilic weak polyelectrolytes. Using the SFA （Surface Forces Apparatus） the authors measured force-distance profiles of poly （isoprene）-poly （acrylic acid） block copolymers adsorbed on mica. Also by Atomic Force Microscopy the authors captured single polyelectrolyte molecule adsorbed on a surface. The effect of salt concentration （Cs） and pH upon the height of the brush layers was explored mainly by measuring the forces between two adsorbed polyelectrolyte brushes. At pH = 4 our results are in good agreement with the scaling prediction L0 ∝Cs-1/3 Changing the pH from 4 to 10 causes a remarkable swelling of the polymer layer, but only a weak dependence on salt concentration was detected at the higher pH. This can be attributed to the degree of dissociation, which depends on the local pH value. At low pH the polyelectrolyte chains have a low charge density, while on increasing the pH the degree of dissociation rises, and the increased charge density is followed by swelling of the adsorbed layer. The local concentration of ions in the brush is now greater than that of pH = 4 and approximately equivalent to 0.3 M. So the swelling is only weakly dependent on salt concentration in the range 0.01-1.0 M. The results demonstrate the tunable nature of such self-assembled polyelectroiyte brushes whose height and range of interactions, can be systematically controlled by adjusting the pH and ionic strength of the medium.展开更多
Two new ultrathin multiplayer films have been successfully prepared fi-om Keggin-type heteropoly acids H-4[SiW12O40] and H-3[PMo12O40] with polyelectrolytes PEI, PSS, and PAH, using the electrostatic layer-by-layer se...Two new ultrathin multiplayer films have been successfully prepared fi-om Keggin-type heteropoly acids H-4[SiW12O40] and H-3[PMo12O40] with polyelectrolytes PEI, PSS, and PAH, using the electrostatic layer-by-layer self-assembly, technique. The XR results reveal their film thickness at nanoscale (similar to 20 nm). According to the AFM images, it is believed that the surface roughness (rough degree of film surface) of the polyelectrolyte-polyoxometalate film greatly depends on the kind of polyoxometalates.展开更多
Based on the layer by layer(Lb L)assembly technology,the nano-scale composite membrane with excellent structure can be prepared by changing the polyelectrolyte and controlling the deposition conditions.Polyamines and ...Based on the layer by layer(Lb L)assembly technology,the nano-scale composite membrane with excellent structure can be prepared by changing the polyelectrolyte and controlling the deposition conditions.Polyamines and phosphate ions(Pi)can be self-organized to form supramolecular systems which could be exploited to stabilize the interfacial architecture.The LbL membrane was made of the positively charged poly(allylamine hydrochloride)(PAH)self-organized with Pi and the negatively charged poly(sodium 4-styrene sulfonate)(PSS)alternatively on top of a poly(acrylonitrile)(PAN)substrate.Compared to the membrane without Pi,the membrane assembled by PAH/Pi improved forward of flux and reduced flux of salt.The concentration of PAH and PSS,deposition time,pH and number of layers showed significant influences on the performance of the membrane.In this experiment,we systematically investigated the preparation conditions and under the optimized conditions the prepared membrane exhibited high water fluxes of 13.5 L m^-2 h^-1 with corresponding salt to water flux,Js/Jv,ratio of 0.07 g L^-1 tested by forward osmosis when DI water as feed solution and 2 mol L^-1 MgCl2 as draw solution.展开更多
Spherical polyelectrolyte brushes （SPBs） consisting of polystyrene （PS） core and poly（2-aminoethyl methacrylate hydrochloride） （PAEMH） shell were prepared by photo-emulsion polymerization. Au nanoparticles （A...Spherical polyelectrolyte brushes （SPBs） consisting of polystyrene （PS） core and poly（2-aminoethyl methacrylate hydrochloride） （PAEMH） shell were prepared by photo-emulsion polymerization. Au nanoparticles （Au-NPs） with controlled size and size distribution were synthesized in situ using SPBs as nanoreactors. Via layer-by-layer deposition technique on the surface of SPBs, nano-composite particles with Au/Ag-NPs bilayer and Au/Ag/Au-NPs trilayer were prepared. The structures of the as-prepared Au/Ag multilayer SPBs were characterized by UV-Vis spectroscopy, TEM, ICP-AES and DLS. The charge reversal of the nano-composite particles observed by zeta potential confirmed the success of layer-by-layer assembly. The Au/Ag-NPs bilayer nano-composite particles showed high catalytic efficiency with an apparent activation energy of about 41.2 kJ/mol in the reduction reaction of 4-nitrophenol to 4-aminophenol in the existence of sodium borohydride monitored. The catalytic activity ofAu/Ag-NPs multilayer SPBs close to that of Au-NPs SPBs and much higher than that of Ag-NPs SPBs reveals its potential applications in cost-effective catalysts with high-performance.展开更多
基金supported by the National Key R&D Program of China(2019YFB1503201)the National Natural Science Foundation of China(52172238,52102304,51902264)+3 种基金the Natural Science Foundation of Shanxi Province(2020JM-093)the Open project of Shaanxi Laboratory of Aerospace Power(2021SXSYS-01-03)the Science Technology and Innovation Commission of Shenzhen Municipality(JCYJ20190807111605472)the Fundamental Research Funds for the Central Universities(3102019JC0005,5000220118)。
文摘SnO_(2)electron transport layer(ETL)is a vital component in perovskite solar cells(PSCs),due to its excellent photoelectric properties and facile fabrication process.In this study,we synthesized a water-soluble and adhesive polyelectrolyte with ethanolamine(EA)and poly-acrylic acid(PAA).The linear PAA was crosslinked by EA,forming a 3D network that stabilized the SnO_(2)nanoparticle dispersion.An organic–inorganic hybrid ETL is developed by introducing the cross-linked PAA-EA into SnO_(2)ETL,which prevents nano particle agglomeration and facilitates uniform SnO_(2)film formation with fewer defects.Additionally,the PAA-EA-modified SnO_(2)facilitated a uniform and compact perovskite film,enhancing the interface contact and carrier transport.Consequently,the PAA-EA-modified PSCs exhibited excellent PCE of 24.34%and 22.88%with high reproducibility for areas of 0.045 and 1.00 cm~2,respectively.Notably,owing to structure reinforce effect of PAA-EA in SnO_(2)ETL,flexible device demonstrated an impressive PCE of 23.34%while maintaining 90.1%of the initial PCE after 10,000 bending cycles with a bending radius of 5 mm.This successful approach of polyelectrolyte reinforced hybrid organic–inorganic ETL displays great potential for flexible,large-area PSCs application.
基金Supported by the National Basic Research Program of China(2015CB655301)the Natural Science Foundation of China(21825803)+2 种基金and the Natural Science Foundation of Jiangsu Province(BK20150063)the Program of Excellent Innovation Teams of Jiangsu Higher Education Institutionsthe Project of Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD).
文摘Thin film composite(TFC) membranes represent a highly promising platform for efficient nanofiltration(NF)processes. However, the improvement in permeance is impeded by the substrates with low permeances. Herein,highly permeable gradient phenolic membranes with tight selectivity are used as substrates to prepare TFC membranes with high permeances by the layer-by-layer assembly method. The negatively charged phenolic substrates are alternately assembled with polycation polyethylenimine(PEI) and polyanion poly(acrylic acid)(PAA)as a result of electrostatic interactions, forming thin and compact PEI/PAA layers tightly attached to the substrate surface. Benefiting from the high permeances and tight surface pores of the gradient nanoporous structures of the substrates, the produced PEI/PAA membranes exhibit a permeance up to 506 L? m-2?h-1?MPa-1, which is ~2–10 times higher than that of other membranes with similar rejections. The PEI/PAA membranes are capable of retaining N 96.1% of negatively charged dyes following the mechanism of electrostatic repulsion. We demonstrate that the membranes can also separate positively and neutrally charged dyes from water via other mechanisms.This work opens a new avenue for the design and preparation of high-flux NF membranes, which is also applicable to enhance the permeance of other TFC membranes.
文摘The authors have investigated the pH and ionic strength response of self-assembled layers formed by adsorption of amphiphilic weak polyelectrolytes. Using the SFA （Surface Forces Apparatus） the authors measured force-distance profiles of poly （isoprene）-poly （acrylic acid） block copolymers adsorbed on mica. Also by Atomic Force Microscopy the authors captured single polyelectrolyte molecule adsorbed on a surface. The effect of salt concentration （Cs） and pH upon the height of the brush layers was explored mainly by measuring the forces between two adsorbed polyelectrolyte brushes. At pH = 4 our results are in good agreement with the scaling prediction L0 ∝Cs-1/3 Changing the pH from 4 to 10 causes a remarkable swelling of the polymer layer, but only a weak dependence on salt concentration was detected at the higher pH. This can be attributed to the degree of dissociation, which depends on the local pH value. At low pH the polyelectrolyte chains have a low charge density, while on increasing the pH the degree of dissociation rises, and the increased charge density is followed by swelling of the adsorbed layer. The local concentration of ions in the brush is now greater than that of pH = 4 and approximately equivalent to 0.3 M. So the swelling is only weakly dependent on salt concentration in the range 0.01-1.0 M. The results demonstrate the tunable nature of such self-assembled polyelectroiyte brushes whose height and range of interactions, can be systematically controlled by adjusting the pH and ionic strength of the medium.
基金This project was financially supported by the National Natural Science Foundation of China (Grant No. 29971006 ).
文摘Two new ultrathin multiplayer films have been successfully prepared fi-om Keggin-type heteropoly acids H-4[SiW12O40] and H-3[PMo12O40] with polyelectrolytes PEI, PSS, and PAH, using the electrostatic layer-by-layer self-assembly, technique. The XR results reveal their film thickness at nanoscale (similar to 20 nm). According to the AFM images, it is believed that the surface roughness (rough degree of film surface) of the polyelectrolyte-polyoxometalate film greatly depends on the kind of polyoxometalates.
基金financial support from the National Natural Science Foundation of China (No. 21476219)Qingdao National Laboratory for Marine Science and Technology (No. QNLM 2016ORP0308)
文摘Based on the layer by layer(Lb L)assembly technology,the nano-scale composite membrane with excellent structure can be prepared by changing the polyelectrolyte and controlling the deposition conditions.Polyamines and phosphate ions(Pi)can be self-organized to form supramolecular systems which could be exploited to stabilize the interfacial architecture.The LbL membrane was made of the positively charged poly(allylamine hydrochloride)(PAH)self-organized with Pi and the negatively charged poly(sodium 4-styrene sulfonate)(PSS)alternatively on top of a poly(acrylonitrile)(PAN)substrate.Compared to the membrane without Pi,the membrane assembled by PAH/Pi improved forward of flux and reduced flux of salt.The concentration of PAH and PSS,deposition time,pH and number of layers showed significant influences on the performance of the membrane.In this experiment,we systematically investigated the preparation conditions and under the optimized conditions the prepared membrane exhibited high water fluxes of 13.5 L m^-2 h^-1 with corresponding salt to water flux,Js/Jv,ratio of 0.07 g L^-1 tested by forward osmosis when DI water as feed solution and 2 mol L^-1 MgCl2 as draw solution.
基金financially supported by the National Natural Science Foundation of China(No.51273063 and 51003028)the Fundamental Research Funds for the Central Universities+1 种基金the Higher School Specialized Research Fund for the Doctoral Program(No.20110074110003)111 Project Grant(No.B08021)
文摘Spherical polyelectrolyte brushes （SPBs） consisting of polystyrene （PS） core and poly（2-aminoethyl methacrylate hydrochloride） （PAEMH） shell were prepared by photo-emulsion polymerization. Au nanoparticles （Au-NPs） with controlled size and size distribution were synthesized in situ using SPBs as nanoreactors. Via layer-by-layer deposition technique on the surface of SPBs, nano-composite particles with Au/Ag-NPs bilayer and Au/Ag/Au-NPs trilayer were prepared. The structures of the as-prepared Au/Ag multilayer SPBs were characterized by UV-Vis spectroscopy, TEM, ICP-AES and DLS. The charge reversal of the nano-composite particles observed by zeta potential confirmed the success of layer-by-layer assembly. The Au/Ag-NPs bilayer nano-composite particles showed high catalytic efficiency with an apparent activation energy of about 41.2 kJ/mol in the reduction reaction of 4-nitrophenol to 4-aminophenol in the existence of sodium borohydride monitored. The catalytic activity ofAu/Ag-NPs multilayer SPBs close to that of Au-NPs SPBs and much higher than that of Ag-NPs SPBs reveals its potential applications in cost-effective catalysts with high-performance.
