Passivation,as a classical surface treatment technique,has been widely accepted in start-of-the-art perovskite solar cells(PSCs)that can effectively modulate the electronic and chemical property of defective perovskit...Passivation,as a classical surface treatment technique,has been widely accepted in start-of-the-art perovskite solar cells(PSCs)that can effectively modulate the electronic and chemical property of defective perovskite surface.The discovery of inorganic passivation compounds,such as oxysalts,has largely advanced the efficiency and lifetime of PSCs on account of its favorable electrical property and remarkable inherent stability,but a lack of deep understanding of how its local configuration affects the passivation effectiveness is a huge impediment for future interfacial molecular engineering.Here,we demonstrate the central-atom-dependent-passivation of oxysalt on perovskite surface,in which the central atoms of oxyacid anions dominate the interfacial oxygen-bridge strength.We revealed that the balance of local interactions between the central atoms of oxyacid anions(e.g.,N,C,S,P,Si)and the metal cations on perovskite surface(e.g.,Pb)generally determines the bond formation at oxysalt/perovskite interface,which can be understood by the bond order conservation principle.Silicate with less electronegative Si central atoms provides strong O-Pb motif and improved passivation effect,delivering a champion efficiency of 17.26%for CsPbI2Br solar cells.Our strategy is also universally effective in improving the device performance of several commonly used perovskite compositions.展开更多
Mg基制氢材料具有来源广泛、反应温和、工艺简单、安全可控、理论产氢量高等优势,是当今的研究热点.本文提出采用高能球磨方法制备Mg-Bi系含氧酸盐Bi_(x)M_(y)O_(z)(M=Ti,V,Cr,Mo,W)复合材料以改善Mg水解制氢性能.本工作研究发现,掺杂Bi...Mg基制氢材料具有来源广泛、反应温和、工艺简单、安全可控、理论产氢量高等优势,是当今的研究热点.本文提出采用高能球磨方法制备Mg-Bi系含氧酸盐Bi_(x)M_(y)O_(z)(M=Ti,V,Cr,Mo,W)复合材料以改善Mg水解制氢性能.本工作研究发现,掺杂Bi_(2)Mo O_(6)的Mg基复合制氢材料具有较好的性能,Mg-7 wt%Bi_(2)Mo O_(6)在298.15 K的最大产氢速率为756.1 m L g^(-1)min(-1).通过引入多壁碳纳米管(CNTs)可以进一步改善Mg-Bi_(2)Mo O_(6)的产氢性能,Mg-7 wt%Bi_(2)Mo O_(6)/CNTs的最大产氢速率达2172.4 m L g^(-1)min(-1),产氢活化能下降至23.6 k J mol^(-1).X光电子能谱(XPS)分析表明Bi_(2)Mo O_(6)/CNTs与Mg在球磨过程中发生固相反应生成Bi单质.密度泛函理论(DFT)计算揭示Bi原子掺杂可改变Mg的局域电荷分布,增强Mg对H_(2)O的吸附能,并降低H_(2)O解离后H原子的吸附能,促进水解反应进行.展开更多
基金Ze Qing Lin and Hui Jun Lian contributed equally to this work.This work was financially supported by National Natural Science Fund for Excellent Young Scholars(52022030)International(Regional)Cooperation and Exchange Projects of the National Natural Science Foundation of China(51920105003)+4 种基金National Natural Science Fund for Distinguished Young Scholars(51725201)National Ten Thousand Talent Program for Young Top-notch Talent,National Natural Science Foundation of China(51902185,51972111)Innovation Program of Shanghai Municipal Education Commission(E00014)Shanghai Engineering Research Center of Hierarchical Nanomaterials(18DZ2252400)The authors also thank the Frontiers Science Center for Materiobiology and Dynamic Chemistry.
文摘Passivation,as a classical surface treatment technique,has been widely accepted in start-of-the-art perovskite solar cells(PSCs)that can effectively modulate the electronic and chemical property of defective perovskite surface.The discovery of inorganic passivation compounds,such as oxysalts,has largely advanced the efficiency and lifetime of PSCs on account of its favorable electrical property and remarkable inherent stability,but a lack of deep understanding of how its local configuration affects the passivation effectiveness is a huge impediment for future interfacial molecular engineering.Here,we demonstrate the central-atom-dependent-passivation of oxysalt on perovskite surface,in which the central atoms of oxyacid anions dominate the interfacial oxygen-bridge strength.We revealed that the balance of local interactions between the central atoms of oxyacid anions(e.g.,N,C,S,P,Si)and the metal cations on perovskite surface(e.g.,Pb)generally determines the bond formation at oxysalt/perovskite interface,which can be understood by the bond order conservation principle.Silicate with less electronegative Si central atoms provides strong O-Pb motif and improved passivation effect,delivering a champion efficiency of 17.26%for CsPbI2Br solar cells.Our strategy is also universally effective in improving the device performance of several commonly used perovskite compositions.
文摘Mg基制氢材料具有来源广泛、反应温和、工艺简单、安全可控、理论产氢量高等优势,是当今的研究热点.本文提出采用高能球磨方法制备Mg-Bi系含氧酸盐Bi_(x)M_(y)O_(z)(M=Ti,V,Cr,Mo,W)复合材料以改善Mg水解制氢性能.本工作研究发现,掺杂Bi_(2)Mo O_(6)的Mg基复合制氢材料具有较好的性能,Mg-7 wt%Bi_(2)Mo O_(6)在298.15 K的最大产氢速率为756.1 m L g^(-1)min(-1).通过引入多壁碳纳米管(CNTs)可以进一步改善Mg-Bi_(2)Mo O_(6)的产氢性能,Mg-7 wt%Bi_(2)Mo O_(6)/CNTs的最大产氢速率达2172.4 m L g^(-1)min(-1),产氢活化能下降至23.6 k J mol^(-1).X光电子能谱(XPS)分析表明Bi_(2)Mo O_(6)/CNTs与Mg在球磨过程中发生固相反应生成Bi单质.密度泛函理论(DFT)计算揭示Bi原子掺杂可改变Mg的局域电荷分布,增强Mg对H_(2)O的吸附能,并降低H_(2)O解离后H原子的吸附能,促进水解反应进行.
