| 1. |
- Guo, Junji, et al.
(författare)
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Unprecedented Electrochromic Stability of a-WO3-x Thin Films Achieved by Using a Hybrid-Cationic Electrolyte
- 2021
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Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 13:9, s. 11067-11077
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Tidskriftsartikel (refereegranskat)abstract
- With large interstitial space volumes and fast ion diffusion pathways, amorphous metal oxides as cathodic intercalation materials for electrochromic devices have attracted attention. However, these incompact thin films normally suffer from two inevitable imperfections: self-deintercalation of guest ions and poor stability of the structure, which constitute a big obstacle toward the development of high-stable commercial applications. Here, we present a low-cost, eco-friendly hybrid cation 1,2-PG-AlCl3 center dot 6H(2)O electrolyte, in which the sputter-deposited a-WO3-x thin film can exhibit both the long-desired excellent open-circuit memory (>100 h, with zero optical loss) and super-long cycling lifetime (similar to 20,000 cycles, with 80% optical modulation), benefiting from the formation of unique Al-hydroxide-based solid electrolyte interphase during electrochromic operations. In addition, the optical absorption behaviors in a-WO3-x caused by host-guest interactions were elaborated. We demonstrated that the intervalence transfers are primarily via the "corner-sharing" related path (W5+ <-> W6+) but not the "edge-sharing" related paths (W4+ <-> W6+ and/or W4+ <-> W5+), and the small polaron/electron transfers taking place at the W-O bond-breaking positions are not allowed. Our findings might provide in-depth insights into the nature of electrochromism and provide a significant step in the realization of more stable, more excellent electrochromic applications based on amorphous metal oxides.
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| 2. |
- Guo, Junji, et al.
(författare)
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Mechanistic Insights into the Coloration, Evolution, and Degradation of NiOx Electrochromic Anodes
- 2018
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Ingår i: Inorganic Chemistry. - : AMER CHEMICAL SOC. - 0020-1669 .- 1520-510X. ; 57:15, s. 8874-8880
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Tidskriftsartikel (refereegranskat)abstract
- NiOx is recognized as the leading candidate for smart window anodes that can dynamically modulate optical absorption, thereby achieving energy efficiency in construction buildings. However, the electrochromic mechanism in NiOx is not yet clear, and the ionic species involved are sometimes ambiguous, particularly in aprotic electrolytes. We demonstrate herein that the "net coloration effect" originates from newly generated high-valence Ni3+/Ni4+ ions during anion-dependent anodization, and the Li+ intercalation/deintercalation only plays a role in modulating the oxidation state of Ni. Unambiguous evidences proving the occurrence of anodization reaction were obtained by both chronoamperometry and cyclic voltammetry. Benefiting from the irreversible polarization of Ni2+ to Ni3+/Ni4+, the quantity of voltammetric charge increases by similar to 38% under the same test conditions, enhancing the corresponding electrochromic modulation by similar to 8%. Strong linkages between the coloration, evolution, and degradation observed in this work provide in-depth insights into the electrocatalytic and electrochromic mechanisms.
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| 3. |
- Guo, Junji, et al.
(författare)
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Prominent Electrochromism Achieved Using Aluminum Ion Insertion/Extraction in Amorphous WO3 Films
- 2018
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Ingår i: The Journal of Physical Chemistry C. - : American Chemical Society (ACS). - 1932-7447 .- 1932-7455. ; 122:33, s. 19037-19043
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Tidskriftsartikel (refereegranskat)abstract
- Although monovalent lithium has been successfully used as a coloring ion in electrochromic applications, it still faces the challenges of low safety, high cost, and limited reserves. Herein, we demonstrate that the amorphous WO3 films intercalated with Al3+ ions could exhibit desired wide optical modulation (similar to 63.0%) and high coloration efficiency (similar to 72.0 cm(2) A(-1), which is >100% higher than that with Li+ or Na+), benefiting from the three-electron redox properties of aluminum. Due to the strong electrostatic force and large atomic weight, the charge exchange processes for Al3+ ions are limited only to the near-surface region and consequently bring about enhanced electrochromic stability. Our findings provide in-depth insights into the nature of electrochromism and also open up a new route toward scalable electrochromic devices using sputtering techniques and earth-abundant materials.
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| 4. |
- Guo, Junji, et al.
(författare)
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Self-Driven Electrochromic Window System Cu/WOx-Al3+/GR with Dynamic Optical Modulation and Static Graph Display Functions
- 2022
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Ingår i: ACS Applied Materials and Interfaces. - : American Chemical Society (ACS). - 1944-8244 .- 1944-8252. ; 14:8, s. 10517-10525
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Tidskriftsartikel (refereegranskat)abstract
- Electrochromic devices with unique advantages of electrical/optical bistability are highly desired for energy-saving and information storage applications. Here, we put forward a self-driven AI-ion electrochromic system, which utilizes WOx films, Cu foil, and graphite rod as electrochromic optical modulation and graph display electrodes, coloration potential supplying electrodes, and bleaching potential supplying electrodes, respectively. The inactive Cu electrode can not only realize the effective Al3+ cation intercalation into electrochromic WOx electrodes but also eliminate the problem of metal anode consumption. The electrochromic WOx electrodes cycled in Al3+ aqueous media exhibit a wide potential window (similar to 1.5 V), high coloration efficiency (36.0 cm(2)/C), and super-long-term cycle stability (>2000 cycles). The dynamic optical modulation and static graph display function can be achieved independently only by switching the electrode connection mode, thus bringing more features to this electrochromic system. For a large-area electrochromic system (10 x 10 cm(2)), the absolute transmittance value in its color-neutral state can reach about 41% (27%) at 633 nm (780 nm) by connecting the Cu and WOx electrodes for 140 s. The original transparent state can be readily recovered by replacing the Cu foil with the graphite rod. This work throws light on next-generation electrochromic applications for optical/thermal modulation, privacy protection, and information display.
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| 5. |
- Guo, Junji, et al.
(författare)
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Vacancy dependent electrochromic behaviors of NiOx anodes : As a single layer and in devices
- 2018
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Ingår i: Solar Energy Materials and Solar Cells. - : ELSEVIER SCIENCE BV. - 0927-0248 .- 1879-3398. ; 178, s. 193-199
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Tidskriftsartikel (refereegranskat)abstract
- Electrochromic(EC), nonstoichiometric NiOx thin films were made by reactive magnetron sputtering at low oxygen flow ratio(i.e., P = O-2/Ar + O-2 < 10%). The results of optical spectral, x-ray diffraction spectrum, and x-ray photoelectron spectroscopy analyses indicate that the samples are oxygen(nickel)-deficient as P <= %4(>=%6), resulting in sub(over)-stoichiometry films. Spectroelectrochemical measurements show that the EC effect of NiOx in nonaqueous PC - LiClO4 electrolyte is direct correlation with the nickel vacancy concentration in films, while that in the aqueous KOH solution is nearly uninfluenced upon the change in stoichiometry as P >= %4. The films deposited at P = 6% exhibit higher coloration efficiency of - 25.3 cm(2)C(-1), larger ionic diffusion coefficient of - 2.84 x 10(-14) m(2)s(-1), and broader EC modulation span of 24% in PC - LiClO4 than the other ones. Based upon these values, EC devices featuring a WO3/PMMA - PC - LiClO4/NiOx structure and excellent performances were fabricated. We demonstrated that the nickel anodization should be responsible for the initial "activation" phenomena, which decreases(increases) the number of oxygen(nickel) vacancies. Moreover, the cause of degradation resulting from Li+-ion trapping in the IS layer was also clarified. This work provides a general framework for studying and designing superior EC devices, experimentally as well as theoretically.
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| 6. |
- Pham, Ngan Hoang, et al.
(författare)
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High thermoelectric power factor of p-type amorphous silicon thin films dispersed with ultrafine silicon nanocrystals
- 2020
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Ingår i: Journal of Applied Physics. - : AIP Publishing. - 0021-8979 .- 1089-7550. ; 127:24
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Tidskriftsartikel (refereegranskat)abstract
- Silicon, a candidate as an abundant-element thermoelectric material for low-temperature thermal energy scavenging applications, generally suffers from rather low thermoelectric efficiency. One viable solution to enhancing the efficiency is to boost the power factor (PF) of amorphous silicon (a-Si) while keeping the thermal conductivity sufficiently low. In this work, we report that PF >1 m Wm−1 K−2 is achievable for boron-implanted p-type a-Si films dispersed with ultrafine crystals realized by annealing with temperatures ≤600 °C. Annealing at 550 °C initiates crystallization with sub-5-nm nanocrystals embedded in the a-Si matrix. The resultant thin films remain highly resistive and thus yield a low PF. Annealing at 600 °C approximately doubles the density of the sub-5-nm nanocrystals with a bimodal size distribution characteristic and accordingly reduces the fraction of the amorphous phase in the films. Consequently, a dramatically enhanced electrical conductivity up to 104 S/m and hence PF > 1 m Wm−1 K−2 measured at room temperature are achieved. The results show the great potential of silicon in large-scale thermoelectric applications and establish a route toward high-performance energy harvesting and cooling based on silicon thermoelectrics.
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| 7. |
- Wu, Yue, et al.
(författare)
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Photoswitching between black and colourless spectra exhibits resettable spatiotemporal logic
- 2016
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Ingår i: Materials Horizons. - : Royal Society of Chemistry. - 2051-6347 .- 2051-6355. ; 3:2, s. 124-129
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Tidskriftsartikel (refereegranskat)abstract
- Logic is the key to computing. Traditionally, logic devices have been fabricated by the top-down approach, whose dimensions are drastically limited. The ultimate goal is to use molecular tailorability to design logics using the "bottom-up'' approach. Here we report an unprecedented photochromic molecule that undergoes unimolecular logic switching when excited anywhere in the entire UV-visible spectrum, thus a bottom-up, all-photonic, molecular logic gate. Specifically, these molecular photonic logics embedded in the polymer thin films function as the "AND'' or "OR'' gate at different temporal responses. To achieve high information-processing density, moreover, a ternary flip-flap-flop gate is realized in the molecular logic because the fact that this photochromic molecule can be photoswitched anywhere in its UV-vis spectrum enabled three different lasers (532, 473, and 561 nm) as the inputs to deliver the complex logic optical outputs.
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