有机有机金属卤化物钙钛矿太阳能电池（PSC）果其低老本战下功率转换效力（PCE）而受到普遍闭注，陈江持策隐现出潜在的照臧志刚中由自下商业价钱。电子传输层（ETL）对于真现晃动下效的许宗祥J下效正置器件起着至关尾要的熏染感动。TiO₂战SnO₂ETL已经普遍操做于老例PSC中。晃动化教惑SnO₂纳米粒子的钙钛团团聚团聚团聚赫然降降器件正在批次间的重现性，那可能会妨碍其商业操做。矿太此外，电池多种的总SnO₂ETL借存正在氧空地（O_V）缺陷，键协展现出较好的同迷体载载流子提与战传输才气。除了ETL中，而上下效SnO₂基PSC的流操略质料牛真现借下度依靠于钙钛矿薄膜的量量。除了ETL战钙钛矿层中，陈江持策为了最小化界里战体相非辐射复开益掉踪，照臧志刚中由自下调节界里玄色常尾要的许宗祥J下效。钙钛矿战SnO₂薄膜的晃动化教惑埋底界里有良多缺陷，那些缺陷会妨碍载流子的提与，导致界里电荷堆散战界里非辐射复开。可是，仅经由历程正在钙钛矿薄膜中减进增减剂份子或者正在埋底界里处引进界里改性剂，很易同时处置上述问题下场战真现总体载流子操持。

鉴于此，重庆小大教陈江照钻研员、臧志刚教授及北边科技小大教许宗祥副教授等人提出了一种由多种化教键协同迷惑的自下而上的总体载流子操持策略，以最小大限度天削减下效钙钛矿太阳能器电池的体相战界里能量益掉踪。该策略是经由历程将露有歉厚夷易近能团（-CF₃、–NH₂–C=NH₂⁺战Cl^-）的4-三氟甲基苯甲脒盐酸盐（TBHCl）直接减进到SnO₂胶体溶液中去真现的，而且借将仅露有-CF₃的三氟甲苯（BTF）战仅露有甲脒阳离子战Cl^-阳离子的苯甲脒盐酸盐（BHCl）用为易刁易比份子，以掀收目的份子中每一个夷易近能团的功能。下场批注，F战Cl^-皆可能经由历程与Sn⁴⁺配位钝化SnO₂中的氧空地战/或者已经配位Sn^4＋缺陷，但前者比后者更实用。F可能经由历程与FA⁺组成氢键去抑制阳离子迁移战调节结晶，而且可能经由历程与Pb²⁺配位去钝化铅缺陷。–NH₂–C=NH₂⁺战Cl^-可分说经由历程与钙钛矿组成离子键战/或者静电相互熏染感动去钝化阳离子战卤素阳离子空地缺陷。总之，目的份子中的各个夷易近能团各司其职，提醉了卓越的协同熏染感动，从而真现了多键迷惑的自下而上的总体载流子操持。经由历程TBHCl改性，抑制了SnO₂纳米粒子的团聚、钝化了ETL中的氧空地缺陷战钙钛矿薄膜中的缺陷战释放了钙钛矿膜中的推伸应变，从而将PCE从21.28%后退到23.40%。散漫PEAI钝化，效力进一步后退到23.63%。TBHCl改性器件具备劣秀的热战干度晃动性。该工做为斥天由多种化教键协同迷惑的自下而上的总体载流子操持策略去提降器件的效力战晃动性提供了借鉴，为钙钛矿太阳能电池的商业化操做奠基了坚真的底子。

Fig. 1.(a) Schematic illustration of multiple-chemical-bond-induced bottom-up holistic modification based on TBHCl. (b) Sn 3dand (c) O 1sXPS spectra of the SnO₂films without or with modifiers. ¹⁹F NMR spectra of the SnO₂solutions without and with (d) BTF and (e) TBHCl. ¹H NMR spectra of the SnO₂solutions without and with (f) BTF and (g) TBHCl. (h) FTIR spectra of SnO₂, SnO₂-TBHCl film, and pure TBHCl in the range of 1000-1200 cm^-1. (i) Pb 4fXPS spectra of the perovskite films prepared on pristine SnO₂and modified SnO₂with BTF, BHCl and TBHCl. (j) ¹⁹F NMR spectra of TBHCl, TBHCl+PbI₂and TBHCl+FAI. (k) ¹H NMR spectra of TBHCl, TBHCl+PbI₂, TBHCl+FAI, and FAI.

Fig. 2.(a) Electrostatic potential map of BTF, BHCl and TBHCl molecules. (b) Binding energies (E_b) between the O_Vdefects in SnO₂, iodine vacancy and FA vacancy defects in FAPbI₃in contact with BTF, BHCl and TBHCl molecules. Optimized structures of SnO₂surface containing O_Vdefects (c) without and with (d) BTF, (e) BHCl, and (f) TBHCl. Optimized structures of FAPbI₃ surface containing iodine vacancy defects (g) without and with (h) BTF, (i) BHCl, and (j) TBHCl. Optimized structures of FAPbI₃surface containing FA vacancy defects (k) without and with (l) BTF, (m) BHCl, and (n) TBHCl.

Fig. 3. DLS spectra of fresh and aged (a) SnO₂, (b) SnO₂-BTF, (c) SnO₂-BHCl and (d) SnO₂-TBHCl. (e) Current-voltage curves for the devices with the structure of ITO/SnO₂without or with modifiers/Ag. The ITO and PCBM stand for the indium-tin oxide-coated glass substrate and phenyl-C61-butyric acid methyl ester layer, respectively. (f) Electron mobility of the electron-only devices with the structure of ITO/PCBM/SnO₂without and with BTF, BHCl and TBHCl/PCBM/Ag. (g) XRD for the control, BTF-, BHCl- and the TBHCl-modified perovskite films. GIXRD patterns with different ωvalues (0.5~1.5) for (h) control, (i) BTF-, (j) BHCl-, and (k) TBHCl-modified perovskite films. (l) The d-spacing value of the (211) plane as a function of grazing incidence angle for the control, BTF-, BHCl- and the TBHCl-modified perovskite films.

Fig. 4. Top-view SEM images of (a) control, (b) BTF-, (c) BHCl-, and (d) TBHCl-modified perovskite films. The scale bar is 1 μm. PL mapping images of (e) glass/perovskite, (f) glass/BTF/perovskite, (g) glass/BHCl/perovskite and (h) glass/TBHCl/perovskite films. (i-l) Current-voltage curves for the electron-only devices which was composed of ITO/SnO₂without or with modifiers /perovskite/PCBM/BCP/Ag.

Fig. 5. (a) TRPL spectra of the perovskite films based on the pristine SnO₂and SnO₂modified with BTF, BHCl, and TBHCl. Transient reflection kinetics for the perovskite films deposited on (b) SnO₂, (c) SnO₂-BTF, (d) SnO₂-BHCl and (e) SnO₂-TBHCl ETLs. (f) TPC and (g) TPV decay curves of the PSCs based on SnO₂, BTF-, BHCl- and TBHCl-modified ETLs. (h) EIS measurement of the devices based on control, BTF, BHCl, and TBHCl ETLs. The inset shows equivalent circuit of the device. (i) The light-intensity dependence of V_OCcurves for the control and modified devices.

Fig. 6. (a) J_SC, (b) V_OC, (c) FF and (d) PCE of the control and PSCs based on the optimal concentration of BTF, BHCl and TBHCl. J-Vcharacteristics of the best-performing PSCs based on (e) control, (f) BTF, (g) BHCl and (h) TBHCl. (i) J-Vcurves of the champion TBHCl modified device with PEAI post-treatment. (j) Steady state output performance of the champion PSCs without and with BTF, BHCl and TBHCl modification. (k) Thermal stability of the unencapsulated PSCs without and with modifiers at 60 ℃ in a N₂-filled glove box. (l) Humidity stability test of unencapsulated PSCs without and with modifiers aged under a relative humidity of 15-25% at room temperature in the dark.

Baibai Liu,¹Ru Li,¹Qixin Zhuang, Xuemeng Yu, Shaokuan Gong, Dongmei He, Qian Zhou, Hua Yang, Xihan Chen, Shirong Lu, Zong-Xiang Xu,* Zhigang Zang* and Jiangzhao Chen*. Bottom-up holistic carrier management strategy induced synergistically by multiple chemical bonds to minimize energy losses for efficient and stable perovskite solar cells. Journal of Energy Chemistry2022, https://doi.org/10.1016/j.jechem.2022.09.037.

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