Pushing up the efficiency of planar perovskite solar cells to 18.2% with organic small molecules as the electron transport layer

Compared to the traditional-architecture perovskite photovoltaic solar cells (n-i-p type), which use metal oxide as electron transport layers (ETLs) and organic semiconducting materials as hole transport layers, the fabrication of metal-oxide-free, solution-processed inverted perovskite solar cells (PSCs) is more desired because of low-temperatures and all-solution-based applications in future commercial PSC modules. In a typical configuration of inverted PSCs, the widely used ETL compound is the fullerene-based phenyl-C61-butyric acid methyl ester (PCBM), which currently is the best organic ETL material. The cost of this compound is very high, and the morphology and electrical properties are very sensitive to experimental conditions. We here propose a new organic ETL material for the replacement of PCBM in inverted PSCs. We demonstrate metal-oxide-free solution-processed inverted PSCs using the n-type sulfur-containing azaacene 10,14-bis(5-(2-ethylhexyl)thiophen-2-yl)-dipyrido[3,2-a:2′,3′-c][1,2,5]thiadiazolo[3,4-i]phenazine (TDTP) as the ETL with a power conversion efficiency of ∼18.2%, which is higher than that of the corresponding non-sulfur-containing azaacene 10,17-bis((triisopropylsilyl)ethynyl)dipyrido[3,2-a:2′,3′-c]quinoxalino[2,3-i]phenazine (PYPH)-based PSCs (up to 9.5%) or PCBM-based PSCs (up to 17.0%). This superior performance is attributed to the stronger interaction between TDTP and the perovskite surface than that between PYPH and the perovskite surface, which is supported by theoretical calculations. Our results show that easily-accessible simple n-type sulfur-containing small molecules are promising ETL candidates to further propel inverted PSCs to practical applications.

[1]  L. Liao,et al.  Improved hole interfacial layer for planar perovskite solar cells with efficiency exceeding 15%. , 2015, ACS applied materials & interfaces.

[2]  Tzung-Fang Guo,et al.  CH3NH3PbI3 Perovskite/Fullerene Planar‐Heterojunction Hybrid Solar Cells , 2013, Advanced materials.

[3]  N. Park,et al.  Lead Iodide Perovskite Sensitized All-Solid-State Submicron Thin Film Mesoscopic Solar Cell with Efficiency Exceeding 9% , 2012, Scientific Reports.

[4]  Ming-Yu Kuo,et al.  Hexaazatrinaphthylene Derivatives: Efficient Electron-Transporting Materials with Tunable Energy Levels for Inverted Perovskite Solar Cells. , 2016, Angewandte Chemie.

[5]  M. Grätzel,et al.  Sequential deposition as a route to high-performance perovskite-sensitized solar cells , 2013, Nature.

[6]  Benlin Hu,et al.  Recent progress in organic resistance memory with small molecules and inorganic–organic hybrid polymers as active elements , 2015 .

[7]  Zong-Liang Tseng,et al.  High efficiency stable inverted perovskite solar cells without current hysteresis , 2015 .

[8]  Peiyang Gu,et al.  Solution-processable thiadiazoloquinoxaline-based donor–acceptor small molecules for thin-film transistors , 2016 .

[9]  Peiyang Gu,et al.  An Azaacene Derivative as Promising Electron-Transport Layer for Inverted Perovskite Solar Cells. , 2016, Chemistry, an Asian journal.

[10]  Peiyang Gu,et al.  An ambipolar azaacene as a stable photocathode for metal-free light-driven water reduction , 2017 .

[11]  Jin Young Kim,et al.  Conjugated polyelectrolyte hole transport layer for inverted-type perovskite solar cells , 2015, Nature Communications.

[12]  Alison E Wendlandt,et al.  Bioinspired aerobic oxidation of secondary amines and nitrogen heterocycles with a bifunctional quinone catalyst. , 2014, Journal of the American Chemical Society.

[13]  M. Grätzel,et al.  A hole-conductor–free, fully printable mesoscopic perovskite solar cell with high stability , 2014, Science.

[14]  Chengyuan Wang,et al.  Synthesis, Structure, and Air-stable N-type Field-Effect Transistor Behaviors of Functionalized Octaazanonacene-8,19-dione. , 2015, Angewandte Chemie.

[15]  Nam-Gyu Park,et al.  Growth of CH3NH3PbI3 cuboids with controlled size for high-efficiency perovskite solar cells. , 2014, Nature nanotechnology.

[16]  Henry J Snaith,et al.  Efficient organometal trihalide perovskite planar-heterojunction solar cells on flexible polymer substrates , 2013, Nature Communications.

[17]  Qi Chen,et al.  Improved air stability of perovskite solar cells via solution-processed metal oxide transport layers. , 2016, Nature nanotechnology.

[18]  Qingfeng Dong,et al.  Giant switchable photovoltaic effect in organometal trihalide perovskite devices. , 2015, Nature materials.

[19]  D. Ginger,et al.  Impact of microstructure on local carrier lifetime in perovskite solar cells , 2015, Science.

[20]  Qichun Zhang,et al.  Linearly Fused Azaacenes: Novel Approaches and New Applications Beyond Field-Effect Transistors (FETs). , 2015, ACS applied materials & interfaces.

[21]  Nripan Mathews,et al.  Low-temperature solution-processed wavelength-tunable perovskites for lasing. , 2014, Nature materials.

[22]  Mingkui Wang,et al.  Amino‐Functionalized Conjugated Polymer as an Efficient Electron Transport Layer for High‐Performance Planar‐Heterojunction Perovskite Solar Cells , 2016 .

[23]  Henk J. Bolink,et al.  Perovskite solar cells employing organic charge-transport layers , 2013, Nature Photonics.

[24]  Bernd Rech,et al.  A mixed-cation lead mixed-halide perovskite absorber for tandem solar cells , 2016, Science.

[25]  W. Jo,et al.  Performance enhancement of planar heterojunction perovskite solar cells by n-doping of the electron transporting layer. , 2015, Chemical communications.

[26]  J. Koenderink Q… , 2014, Les noms officiels des communes de Wallonie, de Bruxelles-Capitale et de la communaute germanophone.

[27]  Yang Yang,et al.  Interface engineering of highly efficient perovskite solar cells , 2014, Science.

[28]  Sergei Tretiak,et al.  High-efficiency solution-processed perovskite solar cells with millimeter-scale grains , 2015, Science.

[29]  Yongbo Yuan,et al.  Non-wetting surface-driven high-aspect-ratio crystalline grain growth for efficient hybrid perovskite solar cells , 2015, Nature Communications.

[30]  Yang Yang,et al.  High-efficiency robust perovskite solar cells on ultrathin flexible substrates , 2016, Nature Communications.

[31]  Gary Hodes,et al.  Perovskite-Based Solar Cells , 2013, Science.

[32]  Fuzhi Huang,et al.  Photovoltaic performance and the energy landscape of CH3NH3PbI3. , 2015, Physical chemistry chemical physics : PCCP.

[33]  Chien-Hung Chiang,et al.  Bulk heterojunction perovskite–PCBM solar cells with high fill factor , 2016, Nature Photonics.

[34]  Yongbo Yuan,et al.  Correlation of energy disorder and open-circuit voltage in hybrid perovskite solar cells , 2016, Nature Energy.

[35]  W. Su,et al.  Quantitative nanoscale monitoring the effect of annealing process on the morphology and optical properties of poly(3-hexylthiophene)/[6,6]-phenyl C61-butyric acid methyl ester thin film used in photovoltaic devices , 2009 .

[36]  Wei Chen,et al.  Efficient and stable large-area perovskite solar cells with inorganic charge extraction layers , 2015, Science.

[37]  Tae Kyu Ahn,et al.  Hysteresis-less inverted CH3NH3PbI3 planar perovskite hybrid solar cells with 18.1% power conversion efficiency , 2015 .

[38]  Chun‐Sing Lee,et al.  Simple fabrication of perovskite solar cells using lead acetate as lead source at low temperature , 2015 .

[39]  Peng Gao,et al.  A molecularly engineered hole-transporting material for efficient perovskite solar cells , 2016, Nature Energy.

[40]  Tsutomu Miyasaka,et al.  Organometal halide perovskites as visible-light sensitizers for photovoltaic cells. , 2009, Journal of the American Chemical Society.

[41]  Nakita K. Noel,et al.  Enhanced photoluminescence and solar cell performance via Lewis base passivation of organic-inorganic lead halide perovskites. , 2014, ACS nano.

[42]  G. Bazan,et al.  New fullerene design enables efficient passivation of surface traps in high performance p-i-n heterojunction perovskite solar cells , 2016 .

[43]  Sung Cheol Yoon,et al.  Efficient CH3NH3PbI3 Perovskite Solar Cells Employing Nanostructured p‐Type NiO Electrode Formed by a Pulsed Laser Deposition , 2015, Advanced materials.

[44]  Sang Il Seok,et al.  High-performance photovoltaic perovskite layers fabricated through intramolecular exchange , 2015, Science.

[45]  M. Grätzel,et al.  Title: Long-Range Balanced Electron and Hole Transport Lengths in Organic-Inorganic CH3NH3PbI3 , 2017 .

[46]  Weiwei Wang,et al.  Inverted planar heterojunction perovskite solar cells employing polymer as the electron conductor. , 2015, ACS applied materials & interfaces.

[47]  Young Chan Kim,et al.  Compositional engineering of perovskite materials for high-performance solar cells , 2015, Nature.

[48]  Timothy L. Kelly,et al.  Perovskite solar cells with a planar heterojunction structure prepared using room-temperature solution processing techniques , 2013, Nature Photonics.

[49]  Zhenggang Huang,et al.  Performance enhancement of fullerene-based solar cells by light processing , 2013, Nature Communications.