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研究背景


钙钛矿太阌™ƒ½ç”‰|± ç”׃ºŽå…¶å…·æœ‰çš„高效率ã€ä½Žæˆæœ¬ã€å·¥è‰ºç®€å•ç­‰ä¼˜åŠ¿è€Œæˆä¸ºç¡…基太阌™ƒ½ç”‰|± æœ€æ½œåœ¨çš„替代者，有机-无机æ‚化钙钛矿电(sh¨´)池的最高光ç”?sh¨´)è{æ¢æ•ˆçŽ‡å·²¾lè¾¾åˆ?/span>25.5%。但是，一般溶液法制备的钙钛矿薄膜存在ç€å¤§é‡çš„晶界，晶界处容易åÅžæˆç¼ºé™øP¼Œé’™é’›çŸ¿å±‚çš„å„¿U缺陷和ä¸å¯æŽ§çš„¾l“晶˜q‡ç¨‹é™åˆ¶äº†å™¨ä»¶æ•ˆçŽ‡å’Œ½E›_®šæ€§çš„˜q›ä¸€æ­¥æå‡ã€‚调控结晶过½E‹å’Œé’化晶界¾~ºé™·æ˜¯æ高钙钛矿太阳能电(sh¨´)池效率和½E›_®šæ€§çš„有效½{–ç•¥åQŒå› æ­¤ï¼Œå¯ÀL‰¾åˆé€‚çš„é’化剂是制备高效½E›_®šé’™é’›çŸ¿å¤ªé˜Œ™ƒ½ç”‰|± çš„关键因素之一ã€?br />

内容½Ž€ä»?/strong>


å—开大学æŽè·ƒé¾™å‰¯æ•™æŽˆ½{?/span>˜q‘æ—¥åœ?/span>ACS Applied Materials & Interfaceså‘表题äØ“(f¨´)â€?/span>Manipulated Crystallization and Passivated Defects for Efficient Perovskite Solar Cells via Addition of Ammonium Iodideâ€?/span>çš„ç ”½I¶è®ºæ–‡ã€‚äØ“(f¨´)了调控钙钛矿的结晶过½E‹å’Œå‡å°‘¾~ºé™·æ€å¯†åº¦ï¼Œæ–‡ç« ç”¨ä¸¤æ­¥æ²‰¿U¯çš„æ–ÒŽ(gu¨©)³•è¯æ˜Žé“늛辅助¾l“晶å¯ä»¥˜q›ä¸€æ­¥æå‡é’™é’›çŸ¿å¤ªé˜³ç”‰|± çš„性能åQŒç¢˜åŒ–铵åQ?/span>NH4IåQ‰çš„加入调控了钙钛矿的æˆæ ¸å’Œæ™¶ä½“生长åQŒä¸­é—´ä½“ x[NH4 ]?[PbI3]x?çš„åÅžæˆå’Œè½¬å˜å¢žå¤§äº†é’™é’›çŸ¿çš„晶¾_’，其中Nä¸?/span>Pbçš„é…ä½ä½œç”¨é’化了钙钛矿中未é…ä½çš„Pb¾~ºé™·åQŒåŒæ—?/span>I能够填补钙钛矿薄膜中çš?/span>I½IÞZ½¾~ºé™·åQŒä»Žè€Œä‹É¾~ºé™·æ€å¯†åº¦å¤§å¤§å‡ž®‘。结晶过½E‹çš„改善和缺é™ïL(f¨¥ng)š„å‡å°‘使器件性能显著æå‡åQŒåŠ å…?/span>NH4I的器件åã^å‡æ•ˆçŽ‡äØ“(f¨´)21.36%åQŒæœ€é«˜æ•ˆçŽ‡è¾¾åˆ?/span>22.15%åQŒåƈ在ä¸åŒæ¹¿åº¦çš„大气环境中表现出良好的稳定性ã€?/span>


å›?/span>1. NH4I作用机ç†å›?/span>


图文å¯ÆD¯»


钙钛矿薄膜的质é‡ç›´æŽ¥å½±å“ç€é’™é’›çŸ¿å¤ªé˜Œ™ƒ½ç”‰|± çš„性能。图2(a-f)昄¡¤ºäº?/span>NH4I处ç†å‰åŽè–„膜的表é¢åŞ貌，SEMåQ?/span>a-båQ‰å’ŒAFMåQ?/span>c-dåQ‰è¡¨æ˜Žäº†ä¸Žå¯¹ç…§ç»„相比åQŒåŠ å…¥äº†NH4I的钙钛矿薄膜晶粒ž®ºå¯¸è¾ƒå¤§åQŒè–„膜更òqÏx•´å…‰æ»‘。加å…?/span>NH4IåŽï¼ŒPbI2的结晶度得到改善åQŒä¸­é—´ç›¸x[NH4 ]?[PbI3]x?çš„åÅžæˆè°ƒæŽ§äº†é’™é’›çŸ¿çš„æˆæ ¸å’Œæ™¶ä½“生长过½E‹ï¼Œ˜q™æ˜¯é’™é’›çŸ¿è–„膜质é‡æå‡çš„主è¦åŽŸå› ã€‚图2e, f昄¡¤ºäº†æ·»åŠ?/span>NH4Iå‰åŽçš„钙钛矿薄膜的开ž®?d¨¡ng)文探针å?/span>(KPFM)囑փ。通过接触ç”?sh¨´)势å?/span>(CPD)æ¥è¡¨å¾è–„膜的表é¢ç”?sh¨´)ä½åQŒåŠ å…?/span>NH4I的钙钛矿膜的CPD值明昑֢žå¤§ï¼Œè¡¨é¢åŠŸå‡½æ•°å€¼éšä¹‹å‡ž®ï¼Œ˜q™ä¹Ÿæ˜¯å™¨ä»¶çš„开压æå‡çš„原因ã€?/span>


å›?/span>2. 加入NH4Iå‰åŽçš„钙钛矿薄膜çš?/span>SEMåQ?/span>a-båQ‰ï¼ŒAFMåQ?/span>c-dåQ‰ï¼ŒKPFMåQ?/span>e-fåQ‰å›¾ã€?/span>


XRDåQˆå›¾3aåQ‰è¿›ä¸€æ­¥å°è¯äº†ä¸Šè¿°¾l“论åQŒé’™é’›çŸ¿æ›´å¼ºçš„è¡ž®„峰表明了钙钛矿更高的薄膜质é‡ï¼ŒåŒæ—¶ç´«å¤–å¸æ”¶å›¾è°±åQˆå›¾3båQ‰æ˜¾½CÞZº†åœ¨çŸ­æ³¢æ®µåQŒåŠ å…¥äº†NH4I的薄膜显½Cºå‡ºæ›´å¼ºçš„光攉™›†èƒ½åŠ›åQŒè¿™ä¹Ÿæ˜¯å™¨äšg短èµ\甉|µå¯†åº¦æå‡çš„主è¦åŽŸå› ã€‚空间é™åˆ¶ç”µ(sh¨´)èïL(f¨¥ng)”µ(sh¨´)‹¹ï¼ˆSCLCåQ‰ï¼ˆå›?/span>3cåQ‰æ˜¾½Cºç»NH4Ié’化åŽï¼Œé™·é˜±å¡«å……é™åˆ¶ç”?sh¨´)压åQ?/span>VTFLåQ‰ä»Ž0.98Vé™ä½Žåˆ?/span>0.63VåQŒç¼ºé™äh€å¯†åº¦ï¼ˆNtåQ‰ä¹Ÿä»?/span>8.44×1015cm-3å‡å°‘åˆ?/span>5.43×1015cm-3。é™ä½Žçš„¾~ºé™·æ€å¯†åº¦å¯ä»¥é€šè¿‡XPSåQˆå›¾3dåQ‰å¾—到è¯å®žï¼Œ¾lé’化åŽè–„膜çš?/span>Pb 4f å³îC½å‘更高结åˆèƒ½å移åQŒè¯æ˜Žäº†Nä¸?/span>Pbçš„é…ä½ä½œç”¨é’化了钙钛矿薄膜中未é…ä½çš„Pb¾~ºé™·åQŒè¿›ä¸€æ­¥è¯å®žäº†NH4I寚w’™é’›çŸ¿ä¸­ç¼ºé™ïL(f¨¥ng)š„é’化作用ã€?/span>



å›?/span>3. NH4Ié’化å‰åŽçš?/span>XRDåQ?/span>aåQ‰ï¼ŒUV-visåQ?/span>båQ‰ï¼ŒSCLCåQ?/span>cåQ‰ï¼ŒXPSåQ?/span>dåQ‰å¯¹æ¯”图ã€?/span>


ä¸ÞZº†å®šé‡ä¼°è®¡é’™é’›çŸ¿è–„膜的¾~ºé™·æ€å¯†åº¦ï¼Œå›?/span>4对电(sh¨´)池进行了å„ç§è¡¨å¾å’Œæ€È»“。图4a昄¡¤ºäº†å™¨ä»¶çš„Vocéšå…‰å¼ºçš„å˜åŒ–。斜率æ‡LåŠ?/span>KBT/q是由界é¢éžè¾ž®„å¤åˆå¼•èµïL(f¨¥ng)š„åQŒç»å¤„ç†çš„器件的nå€ég»Ž1.72下é™åˆ?/span>1.53åQŒè¿›ä¸€æ­¥è¯æ˜?/span>NH4Iå¯ä»¥æœ‰æ•ˆé’化晶界¾~ºé™·òq¶æŠ‘刉™žè¾å°„å¤åˆã€‚æš—æ€?/span>J-VåQˆå›¾4båQ‰ä¹Ÿè¯æ˜ŽåŠ å…¥NH4IåŽé’™é’›çŸ¿å¤ªé˜³ç”‰|± ä¸­ç•Œé¢é‡¾l„凞®‘。图4cçš?/span>Mott-Schottky曲线昄¡¤ºå‡ºé’化åŽå™¨äšg的内¾|®ç”µ(sh¨´)势（VbiåQ‰æ˜Žæ˜¾æå‡ï¼Œè¡¨æ˜Žç”?sh¨´)è·åˆ†ç¦»å’Œæ”¶é›†çš„驱动力更大，有利于获得更高çš?/span>VocåQŒä»Žè€Œæå‡å™¨ä»¶çš„整体性能。此外，利用暗æ¡ä»¶ä¸‹çš„电(sh¨´)化学é˜ÀLŠ—è°?/span>(EIS)åQˆå›¾4dåQ‰ç ”½I¶äº†ç•Œé¢ç”?sh¨´)è·è½¬ç§»åŠ¨åŠ›å­¦ã€‚加å…?/span>NH4I的装¾|®ä¼ è¾“电(sh¨´)阻（RtråQ‰ç”±51.19Ωå‡å°‘åˆ?/span>34.14ΩåQŒå¤åˆç”µ(sh¨´)阻（RreåQ‰ç”±770Ω增加åˆ?/span>1444ΩåQ?/span>Rtrçš„é™ä½Žå’ŒRre的增加表æ˜?/span>NH4I的加入æ高了ç”?sh¨´)è·æå–能力åQŒæœ‰æ•ˆæŠ‘制è²ä½“çš„é‡ç»„ã€?/span>


å›?/span>4. åQ?/span>aåQ‰åŠ å…?/span>NH4Iå‰åŽçš„开压éšå…‰å¼ºå˜åŒ–的曲¾U¿å›¾ã€?/span>NH4I处ç†å‰åŽçš„æš—æ€?/span>J-VåQ?/span>båQ‰ï¼ŒMott?SchottkyåQ?/span>cåQ‰ï¼ŒEISåQ?/span>dåQ‰å¯¹æ¯”图ã€?/span>

å›?/span>5å¯ÒŽ(gu¨©)¯”了ç»NH4Ié’化å‰åŽçš„器件性能。加å…?/span>NH4IåŽå™¨ä»¶åã^å‡æ•ˆçŽ‡ä»Ž20.12%æå‡åˆ?/span>21.36%åQŒæœ€é«˜æ•ˆçŽ‡äØ“(f¨´) 22.15åQ…（RSåQ‰å’Œ22.10åQ…（FSåQ‰ï¼ŒJSCä¸?/span>24.54 mA / cm2åQ?/span>VOCä¸?/span>1.14 VåQ?/span>FFæ˜?/span>79.4åQ…。从J-V曲线å’?/span>EQE集æˆèŽ·å¾—çš?/span>JSC的差异å°äº?/span>3åQ…。此外，300sçš?/span>MPP跟踪表明了器件的优异½E›_®šæ€§ã€?/span>


å›?/span>5. åQ?/span>aåQ‰åŠ å…?/span>NH4IåŽå™¨ä»¶çš„最高效率的J-V曲线ã€?/span>NH4I处ç†å‰åŽçš?/span>EQEåQ?/span>båQ‰æ•ˆçŽ‡åˆ†å¸ƒç®±¾U¿å›¾åQ?/span>cåQ‰ã€‚（dåQ‰åŠ å…?/span>NH4I的电(sh¨´)池在最大功率点å¤?/span>300s内的MPP˜q½è¸ªã€?/span>


作者简�/span>


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  å—开大学ç”?sh¨´)å­ä¿¡æ¯ä¸Žå…‰å­¦å·¥½E‹å­¦é™¢å‰¯æ•™æŽˆåQŒåšå£«ç”Ÿå¯¼å¸ˆã€‚曾入选天‹z¥å¸‚‹¹·å¤–高层‹Æ¡ähæ‰é’òq´é¡¹ç›®ï¼Œ‹Æ§ç›ŸçŽ›ä¸½å±…里学者，担ä“Q国家é‡ç‚¹ç ”å‘计划è¯ùN¢˜è´Ÿè´£äººï¼Œå›½å®¶è‡ªç„¶¿U‘学基金函评专家ã€?/span>2012òq?/span>3月获得韩国科学技术研½I‰™™¢åšå£«å­¦ä½åQ?/span>KIST/USTåQ‰ï¼Œä¹‹åŽåœ¨ç¾Žå›½åŠ å·žå¤§å­?/span>-圣è„P戈分æ ?/span>(UCSD)和西ç­ç‰™å›½å®¶ç ”究é™?/span>(CSIC)从事åšå£«åŽç ”½IÓž¼Œòq¶å…ˆåŽåœ¨è‹±å›½ç‰›æÓ|大学克拉伦登实验室（2015åQ‰å’Œå‰‘桥大学å¡æ–‡˜qªè®¸å®žéªŒå®¤ï¼ˆ2018åQ‰ä½œè®‰K—®ç ”究ã€?/span>2016òq?/span>10月，加入å—开大学ç”?sh¨´)å­ä¿¡æ¯ä¸Žå…‰å­¦å·¥½E‹å­¦é™¢ã€‚ç›®å‰ä¸»æŒå›½å®‰™‡ç‚¹ç ”å‘计划项目课题，‹Æ§ç›Ÿâ€?/span>地åã^¾U?/span>2020â€?/span>™å¹ç›®åQŒå›½å®¶è‡ªç„¶ç§‘学基金é¢ä¸Šé¡¹ç›®ç­‰å›½å®¶æˆ–çœéƒ¨çñ”¿U‘ç ”™å¹ç›®6™åV€‚主è¦ä»Žäº‹çº³¾c›_…‰ç”‰|料与器äšg领域研究åQŒç›®å‰ä¸“注于钙钛矿太阳电(sh¨´)池，钙钛çŸ?/span>/晶硅两端å å±‚甉|± åQŒé’™é’›çŸ¿å•æ™¶æ料与器ä»Óž¼ŒæŸ”性能æºç”µ(sh¨´)å­ç­‰æ–¹å‘研究。曾获得塑料衬底柔性染料æ•åŒ–太阳电(sh¨´)池最高效çŽ?/span>8.55%åQ›èŽ·å¾—全辊涂制备的钙钛矿太阳甉|± æœ€é«˜æ•ˆçŽ?/span>12.34%åQ›åˆ¶å¤‡å‡ºé¦–颗钙钛矉K‡å­ç‚¹¾l“，òq¶å‘现其室温下电(sh¨´)å­¦é‡å­å¹²æ¶‰çŽ°è±¡ï¼›åœ?/span>Energy & Environmental ScienceåQ?/span>Nature CommunicationsåQ?/span>Nano LettersåQ?/span>Nano EnergyåQ?/span>Advanced Functional Materials½{‰é«˜æ°´åã^期刊å‘表学术论文60多篇åQ›ç”³è¯·ä¸­å›½å‘明专åˆ?/span>18™å¹ï¼Œå·²æŽˆæƒç¾Žå›½ã€éŸ©å›½ã€?/span>PCT专利ã€ä¸­å›½ç­‰å‘明专利5™åV€‚æ‹…ä»?/span>Energy & Environmental Science, Advanced Energy Materials½{?/span>30多ç§å­¦æœ¯æ‚志审稿人；担ä“QNano Convergence期刊åQ?/span>Springer Nature出版½C¾ï¼‰(j¨ª)¾~–委ã€?/span>


æŽè·ƒé¾™å‰¯æ•™æŽˆä¸»é¡µ:
https://ceo.nankai.edu.cn/szll/gdzbmqjyjsyjs/lyl.htm


原文链接

https://doi.org/10.1021/acsami.1c05903

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