The performance of proton exchange membrane fuel cells is heavily dependent on the microstructure of electrode catalyst especially at low catalyst loadings.This work shows a hybrid electrocatalyst consisting of PtNi-W...The performance of proton exchange membrane fuel cells is heavily dependent on the microstructure of electrode catalyst especially at low catalyst loadings.This work shows a hybrid electrocatalyst consisting of PtNi-W alloy nanocrystals loaded on carbon surface with atomically dispersed W sites by a two-step straightforward method.Single-atomic W can be found on the carbon surface,which can form protonic acid sites and establish an extended proton transport network at the catalyst surface.When implemented in membrane electrode assembly as cathode at ultra-low loading of 0.05 mgPt cm^(−2),the peak power density of the cell is enhanced by 64.4%compared to that with the commercial Pt/C catalyst.The theoretical calculation suggests that the single-atomic W possesses a favorable energetics toward the formation of*OOH whereby the intermediates can be efficiently converted and further reduced to water,revealing a interfacial cascade catalysis facilitated by the single-atomic W.This work highlights a novel functional hybrid electrocatalyst design from the atomic level that enables to solve the bottle-neck issues at device level.展开更多
Perovskite crystal facets greatly impact the performance and stability of their corresponding photovoltaic devices.Compared to the(001)facet,the(011)facet yields better photoelectric properties,including higher conduc...Perovskite crystal facets greatly impact the performance and stability of their corresponding photovoltaic devices.Compared to the(001)facet,the(011)facet yields better photoelectric properties,including higher conductivity and enhanced charge carrier mobility.Thus,achieving(011)facet-exposed films is a promising way to improve device performance.However,the growth of(011)facets is energetically unfavorable in FAPbI_(3) perovskites due to the influence of methylammonium chloride additive.Here,1-butyl-4-methylpyridinium chloride([4MBP]Cl)was used to expose(011)facets.The[4MBP]^(+)cation selectively decreases the surface energy of the(011)facet enabling the growth of the(011)plane.The[4MBP]^(+)cation causes the perovskite nuclei to rotate by 45°such that(011)crystal facets stack along the out-of-plane direction.The(011)facet has excellent charge transport properties and can achieve better-matched energy level alignment.In addition,[4MBP]Cl increases the activation energy barrier for ion migration,suppressing decomposition of the perovskite.As a result,a small-size device(0.06 cm2)and a module(29.0 cm2)based on exposure of the(011)facet achieved power conversion efficiencies of 25.24%and 21.12%,respectively.展开更多
The power conversion efficiency(PCE)for perovskite solar cells(PSCs)now reaches 25.2%[1].However,the perovskite materials have complex compositions and variable phases,calling for suitable characterization techniques ...The power conversion efficiency(PCE)for perovskite solar cells(PSCs)now reaches 25.2%[1].However,the perovskite materials have complex compositions and variable phases,calling for suitable characterization techniques to investigate the underlying operation and degradation mechanism.展开更多
The long-term stability issue of halide perovskite solar cells hinders their commercialization.The residual stress-strain affects device stability,which is derived from the mismatched thermophysical and mechanical pro...The long-term stability issue of halide perovskite solar cells hinders their commercialization.The residual stress-strain affects device stability,which is derived from the mismatched thermophysical and mechanical properties between adjacent layers.In this work,we introduced the Rb_(2)CO_(3)layer at the interface of SnO_(2)/perovskite with the hierarchy morphology of snowflake-like microislands and dendritic nanostructures.With a suitable thermal expansion coefficient,the Rb_(2)CO_(3)layer benefits the interfacial stress relaxation and results in a compressive stress-strain in the perovskite layer.Moreover,reduced nonradiative recombination losses and optimized band alignment were achieved.An enhancement of open-circuit voltage from 1.087 to 1.153 V in the resultant device was witnessed,which led to power conversion efficiency(PCE)of 22.7%(active area of 0.08313 cm^(2))and 20.6%(1 cm2).Moreover,these devices retained 95%of its initial PCE under the maximum power point tracking(MPPT)after 2700 h.It suggests inorganic materials with high thermal expansion coefficients and specific nanostructures are promising candidates to optimize interfacial mechanics,which improves the operational stability of perovskite cells.展开更多
It is challenging to improve the long-term stability of perovskite solar cells(PSCs) without sacrificing efficiency. The perovskite absorbers degrade from the film surface/interfaces, which follows entangled mechanism...It is challenging to improve the long-term stability of perovskite solar cells(PSCs) without sacrificing efficiency. The perovskite absorbers degrade from the film surface/interfaces, which follows entangled mechanisms that have not been fully revealed yet.Herein, we decouple and elaborate two distinctive pathways regarding film degradation based on FACsPbI3perovskites.Moreover, a dual interfacial modification strategy has been developed for improving the material’s intrinsic stability, thus leading to the film degrading in a more retardant pathway. The corresponding PSCs achieve a stable power output efficiency of 23.75%.More importantly, the unencapsulated PSCs devices retain over 93% of their initial PCE after the maximum power point(MPP)tracking under the continuous 1-sun illumination and show significantly improved stability after aged under the thermal treatment or stored in ambient atmosphere for over 1500 hours without obvious PCE decay. This work shows the importance of modulating the degradation pathway on stability improvement, and at the same time, proposes a strategy for designing perovskite-based optoelectronics with excellent performance and stability.展开更多
基金Y.Li acknowledges the financial support from the National Natural Science Foundation of China(No.52171199)X.Ke acknowledges the financial support from the National Natural Science Foundation of China(No.12074017).
文摘The performance of proton exchange membrane fuel cells is heavily dependent on the microstructure of electrode catalyst especially at low catalyst loadings.This work shows a hybrid electrocatalyst consisting of PtNi-W alloy nanocrystals loaded on carbon surface with atomically dispersed W sites by a two-step straightforward method.Single-atomic W can be found on the carbon surface,which can form protonic acid sites and establish an extended proton transport network at the catalyst surface.When implemented in membrane electrode assembly as cathode at ultra-low loading of 0.05 mgPt cm^(−2),the peak power density of the cell is enhanced by 64.4%compared to that with the commercial Pt/C catalyst.The theoretical calculation suggests that the single-atomic W possesses a favorable energetics toward the formation of*OOH whereby the intermediates can be efficiently converted and further reduced to water,revealing a interfacial cascade catalysis facilitated by the single-atomic W.This work highlights a novel functional hybrid electrocatalyst design from the atomic level that enables to solve the bottle-neck issues at device level.
基金This work was funded by the European Union’s Horizon 2020 program,through a FET Proactive research and innovation action under grant agreement No.101084124(DIAMOND)supported by the 111 Project(B16016),and the Project of Scientific and Technological Support Program in Jiang Su Province(BE2022026-2)+2 种基金K.Z.thanks to the China Scholarship Council(no.202206730056)X.F.Z.thanks to the China Scholarship Council(no.202206730058)R.W.acknowledges the grant(LD22E020002)by the Natural Science Foundation of Zhejiang Province of China.
文摘Perovskite crystal facets greatly impact the performance and stability of their corresponding photovoltaic devices.Compared to the(001)facet,the(011)facet yields better photoelectric properties,including higher conductivity and enhanced charge carrier mobility.Thus,achieving(011)facet-exposed films is a promising way to improve device performance.However,the growth of(011)facets is energetically unfavorable in FAPbI_(3) perovskites due to the influence of methylammonium chloride additive.Here,1-butyl-4-methylpyridinium chloride([4MBP]Cl)was used to expose(011)facets.The[4MBP]^(+)cation selectively decreases the surface energy of the(011)facet enabling the growth of the(011)plane.The[4MBP]^(+)cation causes the perovskite nuclei to rotate by 45°such that(011)crystal facets stack along the out-of-plane direction.The(011)facet has excellent charge transport properties and can achieve better-matched energy level alignment.In addition,[4MBP]Cl increases the activation energy barrier for ion migration,suppressing decomposition of the perovskite.As a result,a small-size device(0.06 cm2)and a module(29.0 cm2)based on exposure of the(011)facet achieved power conversion efficiencies of 25.24%and 21.12%,respectively.
基金supported by National Natural Science Foundation of China(21975028,22011540377)Beijing Municipal Science and Technology Project(Z181100005118002)+2 种基金Beijing Municipal Natural Science Foundation(JQ19008)National Key Research and Development Program of China(2017YFA0206600)the National Natur-al Science Foundation of China(51773045,21772030,51922032,21961160720)for financial support。
文摘The power conversion efficiency(PCE)for perovskite solar cells(PSCs)now reaches 25.2%[1].However,the perovskite materials have complex compositions and variable phases,calling for suitable characterization techniques to investigate the underlying operation and degradation mechanism.
基金National Natural Science Foundation of China,Grant/Award Numbers:52203323,U21A20172,21975028,52172182。
文摘The long-term stability issue of halide perovskite solar cells hinders their commercialization.The residual stress-strain affects device stability,which is derived from the mismatched thermophysical and mechanical properties between adjacent layers.In this work,we introduced the Rb_(2)CO_(3)layer at the interface of SnO_(2)/perovskite with the hierarchy morphology of snowflake-like microislands and dendritic nanostructures.With a suitable thermal expansion coefficient,the Rb_(2)CO_(3)layer benefits the interfacial stress relaxation and results in a compressive stress-strain in the perovskite layer.Moreover,reduced nonradiative recombination losses and optimized band alignment were achieved.An enhancement of open-circuit voltage from 1.087 to 1.153 V in the resultant device was witnessed,which led to power conversion efficiency(PCE)of 22.7%(active area of 0.08313 cm^(2))and 20.6%(1 cm2).Moreover,these devices retained 95%of its initial PCE under the maximum power point tracking(MPPT)after 2700 h.It suggests inorganic materials with high thermal expansion coefficients and specific nanostructures are promising candidates to optimize interfacial mechanics,which improves the operational stability of perovskite cells.
基金financially supported by the National Natural Science Foundation of China (21975028, 52172182, 22011540377)the Beijing Municipal Natural Science Foundation (JQ19008)。
文摘It is challenging to improve the long-term stability of perovskite solar cells(PSCs) without sacrificing efficiency. The perovskite absorbers degrade from the film surface/interfaces, which follows entangled mechanisms that have not been fully revealed yet.Herein, we decouple and elaborate two distinctive pathways regarding film degradation based on FACsPbI3perovskites.Moreover, a dual interfacial modification strategy has been developed for improving the material’s intrinsic stability, thus leading to the film degrading in a more retardant pathway. The corresponding PSCs achieve a stable power output efficiency of 23.75%.More importantly, the unencapsulated PSCs devices retain over 93% of their initial PCE after the maximum power point(MPP)tracking under the continuous 1-sun illumination and show significantly improved stability after aged under the thermal treatment or stored in ambient atmosphere for over 1500 hours without obvious PCE decay. This work shows the importance of modulating the degradation pathway on stability improvement, and at the same time, proposes a strategy for designing perovskite-based optoelectronics with excellent performance and stability.