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金屬鹵鈣鈦礦太陽能電池因其優(yōu)異的性能在光伏領(lǐng)域引起了廣泛的關(guān)注。目前已經(jīng)實(shí)現(xiàn)了高達(dá)26.1%的認(rèn)證效率，該效率能夠與單晶硅電池的效率媲美。然而，差的長(zhǎng)期工作穩(wěn)定性對(duì)鈣鈦礦光伏技術(shù)的商業(yè)化提出了嚴(yán)峻的挑戰(zhàn)。器件中每一個(gè)功能層及其界面與電池的長(zhǎng)期穩(wěn)定性密切相關(guān)。其中，正式p-i-n電池的埋底界面對(duì)制備高效穩(wěn)定鈣鈦礦太陽能電池至關(guān)重要。

鑒于此，陳江照教授和易健宏教授團(tuán)隊(duì)開發(fā)了一種多齒配體增強(qiáng)的螯合策略，通過管理界面缺陷和應(yīng)力來提高埋底界面的穩(wěn)定性。采用雙（2,2,2-三氟乙基）（甲氧羰基甲基）膦酸酯（BTP）修飾埋底界面。BTP中的C=O、P=O和兩個(gè)-CF₃官能團(tuán)協(xié)同鈍化SnO₂表面和鈣鈦礦薄膜底表面的缺陷。而且，BTP修飾有助于減輕界面殘余拉應(yīng)力，促進(jìn)鈣鈦礦結(jié)晶，降低界面能壘。該多齒配體調(diào)控策略適用于不同的鈣鈦礦組分，具有很好的普適性。由于顯著的減少了非輻射復(fù)合和顯著提高的界面接觸，BTP修飾的器件實(shí)現(xiàn)了24.63%的功率轉(zhuǎn)換效率（PCE），這是空氣環(huán)境制備的器件報(bào)道的最高效率之一。未封裝的BTP修飾的器件在10-20%RH環(huán)境中老化3000小時(shí)以上保持初始效率的98.6%。未封裝的BTP修飾的器件加熱老化1728小時(shí)后保持初始效率的84.2%。本工作為通過設(shè)計(jì)多齒螯合配體分子增強(qiáng)埋底界面穩(wěn)定性提供見解與指導(dǎo)。

陳江照教授長(zhǎng)期從事新能源材料與器件研究，共發(fā)表SCI論文104篇，總引用8300余次，H指數(shù)為34。其中，以第一或通訊作者發(fā)表SCI論文82篇，包括1篇Nat. Energy、7篇Adv. Mater.、1篇Energy Environ. Sci.、2篇Angew. Chem. Int. Ed.、4篇Adv. Energy Mater.、4篇Adv. Funct. Mater.、3篇ACS Energy Lett.、1篇Nano-Micro Lett.、2篇Nano Lett.、2篇Nano Energy等，ESI高被引論文19篇，ESI熱點(diǎn)論文4篇，單篇論文最高引用490余次，單篇引用超過100次的論文有16篇，1篇論文入選ACS Energy Letters亮點(diǎn)文章。申請(qǐng)發(fā)明專利12項(xiàng)，其中獲授權(quán)7項(xiàng)。作為主編出版中文專著4部。主持國家自然科學(xué)基金面上、兵團(tuán)重點(diǎn)領(lǐng)域科技攻關(guān)計(jì)劃項(xiàng)目、重慶市自然科學(xué)基金面上、重慶市留學(xué)人員回國創(chuàng)業(yè)創(chuàng)新支持計(jì)劃重點(diǎn)項(xiàng)目等科研項(xiàng)目8項(xiàng)。獲得2023年全球前2%頂尖科學(xué)家、新疆天池英才特聘教授、昆明理工大學(xué)拔尖人才（三層次）、重慶大學(xué)百人、第二屆沙坪壩區(qū)十佳科技青年、2023川渝科技學(xué)術(shù)大會(huì)優(yōu)秀論文特等獎(jiǎng)、重慶市科協(xié)崗位創(chuàng)新爭(zhēng)先行動(dòng)三等獎(jiǎng)、第三屆川渝科技學(xué)術(shù)大會(huì)優(yōu)秀論文二等獎(jiǎng)、2022年Wiley威立中國開放科學(xué)高貢獻(xiàn)作者獎(jiǎng)、2022年Wiley威立中國開放科學(xué)年度作者獎(jiǎng)等獎(jiǎng)勵(lì)與榮譽(yù)10余項(xiàng)。在國內(nèi)外重要學(xué)術(shù)會(huì)議作邀請(qǐng)報(bào)告近20次。擔(dān)任國際/國內(nèi)學(xué)術(shù)會(huì)議大會(huì)主席（1次）、大會(huì)秘書長(zhǎng)（1次）和分會(huì)場(chǎng)主席（4次）。擔(dān)任Nature、Nat. Rev. Phys.、Joule等40余本國際知名學(xué)術(shù)期刊的審稿人。擔(dān)任Nano-Micro Lett.、Carbon Energy、SmartMat、Nano Mater. Sci.、Sci. China-Mater.、eScience和Carbon Neutrality期刊的青年編委及先進(jìn)儲(chǔ)能材料與技術(shù)兵團(tuán)重點(diǎn)實(shí)驗(yàn)室學(xué)術(shù)委員會(huì)委員。

Figure 1.(a) Sn 3d, (b) O 1s, (c) F 1s and (d) P 2p XPS spectra of the SnO₂and SnO₂/BTP films. (e)¹⁹F NMR, and (f-h)¹³C NMR spectra of the SnO₂solutions without and with BTP. (i) TheBinding energies (E_b) between the O_Vdefects in SnO₂in contact with theBTPmolecule. Optimized structure of SnO₂surface containing O_Vdefects.

Figure 2.(a) Optimized structures of FAPbI₃surface containing iodine vacancy defects with BTP. (b) Pb 4f, (c) I 3d, (d) P 2p, (e) O 1s and (f) F 1s XPS spectra of the pure BTP, PbI₂and PbI₂+BTP films. (g) FTIR spectra of the perovskite, BTP+perovskite, and pure BTP films in the range of 1000-1900 cm^-1. (h) The relaxed structure of BTP molecules bridging SnO₂substrate and perovskite through chemical bonds.

Figure 3.AFM imagesof the SnO₂films (a) without and (b) with BTP. (c) XRDpatterns and (d) XRD intensity and FWHM for the control and BTP-modified perovskite films. GIXRD spectra with different ω values (0.5~1.5) of the (e) control, and (f) BTP-modified perovskite films.

Figure 4.Top-view SEM images of the (a) control and (b) BTP-modified perovskite films. The scale bar is 1 μm.AFM images of the perovskite films (c) without and (d) with BTP modification. PL mapping images of the (e) glass/perovskite and (f) glass/BTP/perovskite films. (g) SSPL and (h) TRPL spectra of the glass/without and with BTP/perovskite films measured from the glass side. PVSK stands for the perovskite layer. SCLC for the electron-only devices with the structure of the (i) ITO/SnO₂/perovskite/PCBM/BCP/Ag and (j) ITO/SnO₂/BTP/perovskite/PCBM/BCP/Ag. (k) SSPL and (l) TRPL spectra of the perovskite films deposited on the SnO₂substrates without and with BTP modification.

Figure 5.(a) TPV and (b) TPC decay curves of the PSCs without and with BTP. (c) The light-intensity dependence ofV_OCcurves for the control and BTP-modified devices. (d) Energy level diagram of calculated SnO₂and SnO₂/BTP in comparison with the energy levels of ITO, perovskite films, Spiro-OMeTAD (HTL) and Au. (e) Schematic of the buried interface modified by polydentate ligand BTP.

Figure 6.(a)J-Vcurves of the champion control and BTP modified devices. (b)J-Vcurves of the devices without and with TFE. (c)J-Vcurves of the devices without and with MAC. (d)J-Vcurves of the devices without and with PA. (e)J-Vcurves of best-performing devices without and with BTP using FA_0.85MA_0.15PbI₃composition.(f) The stabilized photocurrent density of best-performing devices without and with BTP using Rb_0.02(FA_0.95Cs_0.05)_0.98PbI_2.91Br_0.03Cl_0.06composition. (g) The stability of the PSCs without and with BTP heated at 65 ℃ in the dark in an N₂-filled glovebox. (h) The stability for the control and BTP-modified devices under a relative humidity (RH) of 10-20% in the dark. (i) The PCE evolution for the control and BTP-modified devices under one sun illumination of 100 mW/cm²provided by white light LED at room temperature in the N₂-filled glovebox.

文章鏈接：

Baibai Liu^#, Qian Zhou^#, Yong Li^#, Yu Chen, Dongmei He*, Danqing Ma, Xiao Han, Ru Li*, Ke Yang, Yingguo Yang, Shirong Lu, Xiaodong Ren*, Zhengfu Zhang, Liming Ding, Jing Feng, Jianhong Yi*, Jiangzhao Chen*. Polydentate ligand reinforced chelating to stabilize buried interface toward high-performance perovskite solar cells.Angewandte Chemie International Edition2024,e202317185.

https://onlinelibrary.wiley.com/doi/10.1002/anie.202317185