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1.
Adv Mater ; : e2407681, 2024 Oct 22.
Artigo em Inglês | MEDLINE | ID: mdl-39439150

RESUMO

Developing high-quality wide bandgap (WBG) perovskites with ≈1.7 eV bandgap (Eg) is critical to couple with silicon and create efficient silicon/perovskite tandem devices. The sufferings of large open-circuit voltage (VOC) loss and unstable power output under operation continuously highlight the criticality to fully develop high-quality WBG perovskite films. In this study, rubidium and thiocyanate as additive regulators in WBG perovskites are incorporated, significantly reducing non-radiative recombination, ion-migration, and phase segregation. The optimized 1.66 eV Eg perovskite solar cells achieved state-of-art 1.3 V VOC (0.36 V deficit), and delivered a stabilized power conversion efficiency of 24.3%, along with good device stability (20% degradation (T80) after over 994 h of operation under 1 sun at ≈65°C). When integrated with a flat front side silicon cell, silicon/perovskite two-terminal tandem device (30% efficient) is obtained with a 1.97 V VOC, and T90 operational lifetime of more than 600 h at room temperature.

2.
Nat Mater ; 23(6): 810-817, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38684883

RESUMO

For halide perovskites that are susceptible to photolysis and ion migration, iodide-related defects, such as iodine (I2) and iodine vacancies, are inevitable. Even a small number of these defects can trigger self-accelerating chemical reactions, posing serious challenges to the durability of perovskite solar cells. Fortunately, before I2 can damage the perovskites under illumination, they generally diffuse over a long distance. Therefore, detrimental I2 can be captured by interfacial materials with strong iodide/polyiodide (Ix-) affinities, such as fullerenes and perfluorodecyl iodide. However, fullerenes in direct contact with perovskites fail to confine Ix- ions within the perovskite layer but cause detrimental iodine vacancies. Perfluorodecyl iodide, with its directional Ix- affinity through halogen bonding, can both capture and confine Ix-. Therefore, inverted perovskite solar cells with over 10 times improved ultraviolet irradiation and thermal-light stabilities (under 85 °C and 1 sun illumination), and 1,000 times improved reverse-bias stability (under ISOS-V ageing tests) have been developed.

3.
Adv Mater ; 36(25): e2401416, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38571375

RESUMO

Ion migration is one of the most critical challenges that affects the stability of metal-halide perovskite solar cells (PSCs). However, the current arsenal of available strategies for solving this issue is limited. Here, novel perovskite active layers following the concept of ordered structures with functional units (OSFU) to intrinsically suppress ion migration, in which a three-dimensional (3D) perovskite layer is deposited by vapor deposition for light absorption and a 2D layer is deposited by solution process for ion inhibition, are constructed. As a promising result, the activation energy of ion migration increases from 0.36 eV for the conventional perovskite to 0.54 eV for the OSFU perovskite. These devices exhibit substantially enhanced operational stability in comparison with the conventional ones, retaining >85% of their initial efficiencies after 1200 h under ISOS-L-1. Moreover, the OSFU devices show negligible fatigue behavior with a robust performance under light/dark cycling aging test (ISOS-LC-1 protocol), which demonstrates the promising application of functional motif theory in this field.

4.
Discov Nano ; 19(1): 39, 2024 Mar 04.
Artigo em Inglês | MEDLINE | ID: mdl-38436896

RESUMO

Organic solar cells (OSCs) are considered as a crucial energy source for flexible and wearable electronics. Pseudo-planar heterojunction (PPHJ) OSCs simplify the solution preparation and morphology control. However, non-halogenated solvent-printed PPHJ often have an undesirable vertical component distribution and insufficient donor/acceptor interfaces. Additionally, the inherent brittleness of non-fullerene small molecule acceptors (NFSMAs) in PPHJ leads to poor flexibility, and the NFSMAs solution shows inadequate viscosity during the printing of acceptor layer. Herein, we propose a novel approach termed polymer-incorporated pseudo-planar heterojunction (PiPPHJ), wherein a small amount of polymer donor is introduced into the NFSMAs layer. Our findings demonstrate that the incorporation of polymer increases the viscosity of acceptor solution, thereby improving the blade-coating processability and overall film quality. Simultaneously, this strategy effectively modulates the vertical component distribution, resulting in more donor/acceptor interfaces and an improved power conversion efficiency of 17.26%. Furthermore, PiPPHJ-based films exhibit superior tensile properties, with a crack onset strain of 12.0%, surpassing PPHJ-based films (9.6%). Consequently, large-area (1 cm2) flexible devices achieve a considerable efficiency of 13.30% and maintain excellent mechanical flexibility with 82% of the initial efficiency after 1000 bending cycles. These findings underscore the significant potential of PiPPHJ-based OSCs in flexible and wearable electronics.

5.
Sci Rep ; 13(1): 16785, 2023 Oct 05.
Artigo em Inglês | MEDLINE | ID: mdl-37798440

RESUMO

As China has entered a new stage of high-quality development, clarifying the mechanism and spatial characteristics of green development for urban agglomerations are critical to sustainable development. Based on the data of 11 major cities in the Harbin-Changchun urban agglomeration (HCUA) from 2010 to 2020, this study constructs an evaluation system of green development index (GDI) is composed of four dimensions, i.e. urban green construction (UGC), industrial green development (IGD), resource and environmental carrying capacity (RECC), and technological innovation support (TIS). Furthermore, using the entropy weight method to obtain the weights of evaluation indicators. And then, the comprehensive index calculation is used to evaluate the GDI. The driving factors of each level of GDI are determined by the Pearson correlation coefficient. The results infer some novel findings as follows: (1) the overall tendency of the GDI of the HCUA has gradually increased from 0.358 in 2010 to 0.379 in 2020 which is at the average level. The dimension of TIS shows the highest rate of contribution while IGD and RECC show a fluctuating trend over the time window. (2) The GDI in the HCUA exhibits a patchy clustering differentiation feature that spreads from the central area to the surrounding areas with a "high in the south and low in the north" pattern. Specifically, Changchun, Harbin, and Daqing form an "inverted triangle" structure in geographical location to drive the green development of neighboring areas. (3) The core cities of the HCUA, Changchun, and Harbin, show a much higher level than the other cities. Jilin and Daqing are at the average level, and besides, the rest of the cities of GDI are at the poor level with significant fluctuations in ranking. (4) There are different driving factors between each level of GDI. For cities with good and average levels should focus on protecting resources and the environment. Meanwhile, cities with poor level of GDI need to improve IGD to optimize the urban green structure. Thus, it is suggested to strengthen the flow of factors and implement differentiated strategies to promote coordinated development and spatial clustering.

6.
Adv Mater ; 35(3): e2207336, 2023 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-36305597

RESUMO

The high trap density (generally 1016 to 1018  cm-3 ) in thin films of organic semiconductors is the primary reason for the inferior charge-carrier mobility and large nonradiative recombination energy loss (ΔEnr ) in organic solar cells (OSCs), limiting improvement in power conversion efficiencies (PCEs). In this study, the trap density in OSCs is efficiently reduced via extending the donor core of nonfullerene acceptors (NFAs) from a heptacyclic unit to a nonacyclic unit. TTPIC-4F with a nonacyclic unit has stronger intramolecular and intermolecular interactions, affording higher crystallinity in thin films relative to its counterpart BTPIC-4F. Thus, the D18:TTPIC-4F-based device achieves a lower trap density of 4.02 × 1015  cm-3 , comparable to some typical high-performance inorganic/hybrid semiconductors, with higher mobility and inhibited charge-carrier recombination in devices. Therefore, the D18:TTPIC-4F-based OSC exhibits an impressive PCE of 17.1% with a low ΔEnr of 0.208 eV, which is the best known value for A-D-A-type NFAs. Therefore, extending the donor core of NFAs is an efficient method for suppressing trap states in OSCs for high PCEs.

7.
Adv Mater ; 34(35): e2203529, 2022 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-35908154

RESUMO

Most methods of depositing perovskite films cannot meet the diverse requirements of real applications such as depositing films on various types of substrates, making patterns with different bandgaps for full-color display. Here, a robust mass transfer method of perovskite films and nanostructures is reported, meeting those requirements, by using an ultrathin branched polyethylenimine as interfacial chemical bonding layers. The transfer-printed perovskite films exhibit comparable morphology, composition, optoelectronic properties, and device performances with the counterparts made by optimized spin-coating methods. The perovskite light-emitting diodes (PeLEDs) using the transfer-printed films show decent external quantum efficiencies of 10.5% and 6.7% for red (680 nm) and sky-blue (493 nm) emissions, which are similar to the devices made by spin-coating. This robust transfer printing method also enables the the preparation of perovskite micropatterns with a high resolution up to 1270 pixels per inch. Horizontally aligned red and sky-blue perovskite microstripes are further obtained through multiple printing processes for white PeLEDs. This work demonstrates a feasible strategy for making perovskite films or micropatterns on various substrates for real applications in full-color display, white LEDs, lasing, etc.

8.
Science ; 377(6605): 531-534, 2022 07 29.
Artigo em Inglês | MEDLINE | ID: mdl-35901131

RESUMO

In halide perovskite solar cells the formation of secondary-phase excess lead iodide (PbI2) has some positive effects on power conversion efficiency (PCE) but can be detrimental to device stability and lead to large hysteresis effects in voltage sweeps. We converted PbI2 into an inactive (PbI2)2RbCl compound by RbCl doping, which effectively stabilizes the perovskite phase. We obtained a certified PCE of 25.6% for FAPbI3 (FA, formamidinium) perovskite solar cells on the basis of this strategy. Devices retained 96% of their original PCE values after 1000 hours of shelf storage and 80% after 500 hours of thermal stability testing at 85°C.

9.
ACS Appl Mater Interfaces ; 14(21): 24583-24591, 2022 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-35580174

RESUMO

A significant challenge facing perovskite narrowband photodetectors is making high-quality and thick enough films. Here, we report a facile one-step spray-coating approach to deposit cesium lead halide perovskite thick films for filterless narrowband photodetectors, which exhibited a specific detectivity of 2.43 × 1010 Jones at 655 nm with an fwhm of 25 nm. We demonstrated that both substrate temperature and deposition time during the spray-coating process are key factors that govern the thickness and morphology of perovskite films. The photodetection behavior was dependent on the film thickness, and the narrowband photoresponse was recorded at a 3.9 µm thickness. We discovered that the internal electric field also plays a critical role in determining the narrowband photoresponse behavior. A distinct photoresponse behavior was observed when respectively applying a reverse bias and a forward bias, which is ascribed to the trade-off between the charge-trapping effect and charge extraction under the internal built-in electric field in different biased conditions. Through changing the halogen composition of perovskites from CsPbCl2Br to CsPbI2Br, the peak position of the narrowband spectral photoresponse was observed to shift from 460 to 660 nm. This study not only offers a controllable spray-coating approach to develop thick perovskite films but also provides an important guidance for the rational design of filterless narrowband photodetectors for practical applications in industrial control, visual imaging, and biological sensing.

10.
ACS Appl Mater Interfaces ; 13(47): 56358-56365, 2021 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-34788529

RESUMO

Solution-processable all-inorganic lead halide perovskites are under intensive attention due to their potential applications in low-cost high-performance optoelectronic devices such as photodetectors. However, solution processing usually generates structural and chemical defects which are detrimental to the photodetection performance of photodetectors. Here, a polymer additive of polyethylene glycol (PEG) was employed to passivate the localized defects in CsPbI2Br films through the Lewis acid-base interaction. The interfacial defects were passivated efficiently by introducing a trace amount of a PEG additive with a concentration of 0.4 mg mL-1 into the CsPbI2Br precursor solution, as suggested by the significantly reduced trap density of state, which was revealed using thermal admittance spectroscopy. Fourier transform infrared spectrum characterization showed that rather than Cs+ or I-, a Lewis acid-base interaction was established between Pb2+ and PEG to passivate the defects in the CsPbI2Br perovskite, which leads to large suppression of noise current. Both specific detectivity and linear dynamic range improved from 4.1 × 109 Jones and 73 dB to 2.2 × 1011 Jones and 116 dB, respectively. Our work demonstrates the feasibility of employing an environmentally stable polymeric additive PEG to passivate defects for high photodetection performance in all-inorganic perovskite photodetectors.

11.
Adv Mater ; 33(48): e2104842, 2021 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-34590357

RESUMO

The intrinsic soft lattice nature of organometal halide perovskites (OHPs) makes them very tolerant to defects and ideal candidates for solution-processed optoelectronic devices. However, the soft lattice results in low stability towards external stresses such as heating and humidity, high density of phonons and strong electron-phonon coupling (EPC). Here, it is demonstrated that the OHPs with unsaturated 4-vinylbenzylammonium (VBA) as organoammonium cations can be polymerized without damaging the perovskite structure and its tolerance to defects. The polymerized perovskites show enhanced stability and flexibility compared to regular three-dimensional and two-dimensional (2D) perovskites. Furthermore, the polymerized 4-vinylbenzylammonium group improves perovskite lattice rigidity substantially, resulting in a reduced non-radiative recombination rate because of suppressed electron-phonon coupling, and enhanced carrier mobility because of suppressed phonon scattering. 2D polymerized perovskite light-emitting diodes (PeLEDs) with strong electroluminescence at room temperature, and quasi-2D PeLEDs with an external quantum efficiency (EQE) of 23.2% and enhanced operation stability are demonstrated. The work has opened a new way of enhancing the intrinsic stability and optoelectronic properties of OHPs.

12.
Artigo em Inglês | MEDLINE | ID: mdl-33435198

RESUMO

Land comprehensive carrying capacity (LCCC) reflects the limits of urban development that the land ground in the spatial area can bear under the constraints of society, economy, resources, and environment. An accurate and objective evaluation of LCCC is of great significance to the rational planning of urban space. Using the entropy method to obtain the weights of evaluation indexes, this study constructed an index system composed of four subsystems, i.e., urban construction (UC), social economy (SE), industry development (ID), and urban ecology (UE). Furthermore, calculating the index of 11 cities for the Harbin-Changchun urban agglomeration (HCUA) to analyze the influence of LCCC from diverse dimensions for the period 2004-2015. Lastly, the spatial and temporal differentiation characteristics between the neighboring units of LCCC were visualized through global and local spatial analysis. The results infer some novel findings as follows. (1) The overall tendency of the LCCC of the HCUA has gradually increased over the time window with the coordination of each subsystem. The urban ecological subsystem shows the highest rate of contribution and the social economy subsystem has the largest increase. Urban construction and industry development have a lower number of hot spot cities and lower clustering characteristics than social economy and urban ecology. (2) The core cities of the HCUA, Changchun and Harbin, demonstrate the reverse trend from 2010 to 2015, which reveals the states of excellent and good carrying capacity, respectively. In contrast, four cities are at the inferior state, and three cities are poor. Prioritizing the promotion of the industry development subsystem should be considered for these seven cities. (3) There is some spatial variation of LCCC in the HCUA, which shows the characteristic of "gradually decreasing from the core city to the surrounding area". Changchun and Jilin are high-high clustering areas that drive Siping from a cold spot to a hot spot. Focusing on the development of secondary growth pole cities, Jilin and Songyuan are forming complementary and mutual reinforcement with the core cities, which has a positive significance in promoting the sustainable development of the regional space of urban agglomeration.


Assuntos
Conservação dos Recursos Naturais , Reforma Urbana , China , Cidades , Análise Espacial , Análise Espaço-Temporal , Urbanização
15.
Sci Bull (Beijing) ; 66(6): 621-636, 2021 Mar 30.
Artigo em Inglês | MEDLINE | ID: mdl-36654432

RESUMO

The power conversion efficiency for single-junction solar cells is limited by the Shockley-Quiesser limit. An effective approach to realize high efficiency is to develop multi-junction cells. These years have witnessed the rapid development of organic-inorganic perovskite solar cells. The excellent optoelectronic properties and tunable bandgaps of perovskite materials make them potential candidates for developing tandem solar cells, by combining with silicon, Cu(In,Ga)Se2 and organic solar cells. In this review, we present the recent progress of perovskite-based tandem solar cells, including perovskite/silicon, perovskite/perovskite, perovskite/Cu(In,Ga)Se2, and perovskite/organic cells. Finally, the challenges and opportunities for perovskite-based tandem solar cells are discussed.

16.
Sensors (Basel) ; 22(1)2021 Dec 30.
Artigo em Inglês | MEDLINE | ID: mdl-35009806

RESUMO

As a revolutionary technology, terrestrial laser scanning (TLS) is attracting increasing interest in the fields of architecture, engineering and construction (AEC), with outstanding advantages, such as highly automated, non-contact operation and efficient large-scale sampling capability. TLS has extended a new approach to capturing extremely comprehensive data of the construction environment, providing detailed information for further analysis. This paper presents a systematic review based on scientometric and qualitative analysis to summarize the progress and the current status of the topic and to point out promising research efforts. To begin with, a brief understanding of TLS is provided. Following the selection of relevant papers through a literature search, a scientometric analysis of papers is carried out. Then, major applications are categorized and presented, including (1) 3D model reconstruction, (2) object recognition, (3) deformation measurement, (4) quality assessment, and (5) progress tracking. For widespread adoption and effective use of TLS, essential problems impacting working effects in application are summarized as follows: workflow, data quality, scan planning, and data processing. Finally, future research directions are suggested, including: (1) cost control of hardware and software, (2) improvement of data processing capability, (3) automatic scan planning, (4) integration of digital technologies, (5) adoption of artificial intelligence.


Assuntos
Inteligência Artificial , Lasers , Engenharia , Indústrias , Luz
17.
Adv Sci (Weinh) ; 7(24): 2002445, 2020 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-33344132

RESUMO

Tailoring the organic spacing cations enables developing new Ruddlesden-Popper (RP) perovskites with tunable optoelectronic properties and superior stabilities. However, the formation of highly crystallized RP perovskites can be hindered when the structure of organic cations become complex. Strategies to regulate crystal growing process and grains quality remain to be explored. In this study, mixing Rb+ ions in precursor solution is reported to significantly promote the crystallinity of phenylethylammonium (PEA+) based RP perovskites without impacting on the major orientation of perovskite grains, which leads to increased power conversion efficiencies from 12.5% to 14.6%. It is found that the added Rb+ ions prefer to accumulate at crystal growing front and form Rb+ ions-rich region, which functions as mild crystal growth inhibitor to retard the absorption and diffusion of organic cations at growing front and hence regulates crystal growing rate. The retarded crystal growth benefits PEA-based RP perovskite films with elevated crystal qualities and prolonged carrier recombination lifetimes. Similar increased crystallinity and photovoltaic performance are achieved in other RP perovskites with non-linear organic cations such as phenylmethylammonium (PMA+), 1-(2-naphthyl)-methanammoniun (NMA+) by adding Rb+ ions, demonstrating using a small amount of growth inhibitor as a general route to regulate crystal growth.

18.
ACS Appl Mater Interfaces ; 12(49): 55064-55071, 2020 Dec 09.
Artigo em Inglês | MEDLINE | ID: mdl-33231418

RESUMO

Planar heterojunction (PHJ) organic photodetectors are potentially more stable than traditional bulk heterojunction counterparts because of the absence of uncontrolled phase separation in the donor and acceptor binary blend system. This work reports a new class of PHJ organic photodetectors based on the medium-band gap fullerene C60 and low-band gap fused-ring non-fullerene acceptor ID-MeIC bilayer structure, which allows a wide range of spectral response tuning across the UV-visible-near-infrared (UV-vis-NIR) region by tailoring individual layer thickness. The C60 layer not only increases the external quantum efficiency at 745 nm by 57% but also reduces dark currents by two orders of magnitude. More importantly, the p-type poly[N,N'-bis(4-butylphenyl)-N,N'-bis(phenyl)-benzi] is found to be the key compound to conduct the layer-by-layer fabrication as combined with n-type ID-MeIC for higher charge extraction efficiency. In light of the above information, PHJ organic photodetectors exhibited a specific detectivity of 6.5 × 1010 Jones to detect NIR light at 745 nm under -0.1 V. The linear dynamic range was estimated to be 80 dB. This work has demonstrated a feasible approach to develop a PHJ architecture with tunable spectral response in the UV-vis-NIR range toward long-term stable organic photodetectors for potential applications in flexible and wearable biomedical sensors.

19.
Nat Chem Biol ; 16(8): 912-919, 2020 08.
Artigo em Inglês | MEDLINE | ID: mdl-32541965

RESUMO

The design and optimization of biosynthetic pathways for industrially relevant, non-model organisms is challenging due to transformation idiosyncrasies, reduced numbers of validated genetic parts and a lack of high-throughput workflows. Here we describe a platform for in vitro prototyping and rapid optimization of biosynthetic enzymes (iPROBE) to accelerate this process. In iPROBE, cell lysates are enriched with biosynthetic enzymes by cell-free protein synthesis and then metabolic pathways are assembled in a mix-and-match fashion to assess pathway performance. We demonstrate iPROBE by screening 54 different cell-free pathways for 3-hydroxybutyrate production and optimizing a six-step butanol pathway across 205 permutations using data-driven design. Observing a strong correlation (r = 0.79) between cell-free and cellular performance, we then scaled up our highest-performing pathway, which improved in vivo 3-HB production in Clostridium by 20-fold to 14.63 ± 0.48 g l-1. We expect iPROBE to accelerate design-build-test cycles for industrial biotechnology.


Assuntos
Vias Biossintéticas/fisiologia , Engenharia Metabólica/métodos , Biologia Sintética/métodos , Vias Biossintéticas/efeitos dos fármacos , Biotecnologia/métodos , Sistema Livre de Células/metabolismo , Redes e Vias Metabólicas/fisiologia , Biossíntese de Proteínas/genética , Biossíntese de Proteínas/fisiologia
20.
Opt Lett ; 45(12): 3325-3328, 2020 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-32538974

RESUMO

Conventional metal-semiconductor-metal (MSM) ultraviolet (UV) detectors have the disadvantage of limited adjustable structural parameters, finite electrical field, and long carrier path. In this Letter, we demonstrate a three-dimensional (3D) MSM structural AlN-based deep-UV (DUV) detector, fabricated through simple trench etching and metal deposition, while flip bonding to the silicon substrate forms a flip-chip 3D-MSM (FC-3DMSM) device. 3D-MSM devices exhibit improved responsiveness and response speed, compared with conventional MSM devices. Time-dependent photoresponse of all devices is also investigated here. The enhanced performance of the 3D-MSM device is to be attributed to the intensified electrical field from the 3D metal electrode configuration and the inhibition of the carrier vertical transport, which unambiguously increases the carrier collection efficiency and migration speed, and thus the responsivity and speed as well. This work should advance the design and fabrication of AlN-based DUV detectors.

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