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1.
ACS Appl Mater Interfaces ; 12(20): 22853-22861, 2020 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-32337968

RESUMO

Numerous trap states and low conductivity of compact TiO2 layers are major obstacles for achieving high power conversion efficiency and high-stability perovskite solar cells. Here we report an effective Na2S-doped TiO2 layer, which can improve the conductivity of TiO2 layers, the contact of the TiO2/perovskite interface, and the crystallinity of perovskite layers. Comprehensive investigations demonstrate that Na cations increase the conductivity of TiO2 layers while S anions change the wettability of TiO2 layers, thus improving the crystallinity of perovskite layers and passivate defects at the TiO2/PVK interface. The synergetic effects of dopants lead to a champion efficiency as high as 21.25% in unencapsulated perovskite solar cells (PSCs), with much-improved stability. Our work provides new insights on anion dopants in TiO2 layers, which is usually neglected in previous reports, and also proposes a simple approach to produce low-cost and high-performance electron transport layers for high-performance PSCs.

2.
iScience ; 21: 217-227, 2019 Nov 22.
Artigo em Inglês | MEDLINE | ID: mdl-31675551

RESUMO

The inorganic metal oxides (IMOs), including titanium dioxide (TiO2) and tin dioxide (SnO2), inevitably induce decomposition of perovskite under UV illumination owing to their photocatalytic activity, and the use of a UV filter will add extra cost and reduce the effective power output. Here, we first reveal that the weak Pb-I bond in I-based perovskite is prone to breakage under UV photocatalysis, leading to serious degradation of the SnO2/perovskite interface. We introduced a chlorine-rich mixed-halide perovskite interlayer (ClMPI), which possesses an excellent tolerance to photocatalysis owing to the strong Pb-Cl bond, between the SnO2 and I-based perovskite. The ClMPI-based device achieves an enhanced efficiency of up to 21.01% (certified 20.17%). Most importantly, the resultant devices can maintain >94% of their initial performance after 180 h under outdoor solar irradiation, >80% after 500 h under UV irradiation, and 500 h under continuous full spectrum illumination at their maximum power points.

3.
Nanotechnology ; 31(8): 085401, 2019 Nov 08.
Artigo em Inglês | MEDLINE | ID: mdl-31703224

RESUMO

The performance of hybrid perovskite solar cells (PSCs) is significantly influenced by the crystallization and morphology of perovskite films. Herein, a novel method of CsPbBr3 quantum dots (QDs) assisted nucleation is applied to prepare high quality solution-processed methylammonium lead iodide (MAPbI3) films by employing CsPbBr3 QDs as an additive into diethyl ether anti-solvent. The appropriate amount of CsPbBr3 QDs can act as effective heterogeneous nucleation centers, leading to the formation of smooth and pinhole-free perovskite films with increased grain size. Furthermore, the growth direction of MAPbI3 grains is regulated by CsPbBr3 QDs, exhibiting preferential orientation of (110) plane. Therefore, the MAPbI3 films with CsPbBr3 QDs modification show reduced defects and increased carrier lifetime. As a result, the champion PSC with a maximum power conversion efficiency (PCE) up to 20.17% is achieved and 85% of its initial PCE is maintained after aging 1000 h at room temperature under a relative humidity of 50%. This work demonstrates a feasible way to prepare high quality perovskite films for optoelectronic applications.

4.
Chemistry ; 25(68): 15516-15524, 2019 Dec 05.
Artigo em Inglês | MEDLINE | ID: mdl-31469453

RESUMO

The separation of acetylene from ethylene is of paramount importance in the purification of chemical feedstocks for industrial manufacturing. Herein, an isostructural series of gallate-based metal-organic frameworks (MOFs), M-gallate (M=Ni, Mg, Co), featuring three-dimensionally interconnected zigzag channels, the aperture size of which can be finely tuned within 0.3 Šby metal replacement. Controlling the aperture size of M-gallate materials slightly from 3.69 down to 3.47 Šcould result in a dramatic enhancement of C2 H2 /C2 H4 separation performance. As the smallest radius among the studied metal ions, Ni-gallate exhibits the best C2 H2 /C2 H4 adsorption separation performance owing to the strongest confinement effect, ranking after the state-of-the-art UTSA-200a with a C2 H4 productivity of 85.6 mol L-1 from 1:99 C2 H2 /C2 H4 mixture. The isostructural gallate-based MOFs, readily synthesized from inexpensive gallic acid, are demonstrated to be a new top-performing porous material for highly efficient adsorption of C2 H2 from C2 H4 .

5.
J Am Chem Soc ; 140(13): 4596-4603, 2018 04 04.
Artigo em Inglês | MEDLINE | ID: mdl-29540058

RESUMO

Research on hydrogen-bonded organic frameworks (HOFs) has been developed for quite a long time; however, those with both established permanent porosities and functional properties are extremely rare due to weak hydrogen-bonding interactions among molecular organic linkers, which are much more fragile and difficult to stabilize. Herein, through judiciously combining the superiority of both the moderately stable coordination bonds in metal-organic frameworks and hydrogen bonds, we have realized a microporous hydrogen-bonded metal-complex or metallotecton framework HOF-21, which not only shows permanent porosity, but also exhibits highly selective separation performance of C2H2/C2H4 at room temperature. The outstanding separation performance can be ascribed to sieving effect confined by the fine-tuning pores and the superimposed hydrogen-bonding interaction between C2H2 and SiF62- on both ends as validated by both modeling and neutron powder diffraction experiments. More importantly, the collapsed HOF-21 can be restored by simply immersing it into water or salt solution. To the best of our knowledge, such extraordinary water stability and restorability of HOF-21 were observed for the first time in HOFs, underlying the bright perspective of such new HOF materials for their industrial usage.

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