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1. Light angle dependence of photothermal properties in oxide and porphyrin thin films for energy-efficient window applications

   https://doi.org/https://doi.org/10.1557/mrc.2020.39  

   1. Lyu M, Lin J (June 2020, MRS communications)

   null (Ed.)

   The photothermal experiments on the incident light angle dependence are carried out using simulated solar light on thin films of both iron oxides (Fe3O4 and Fe3O4@Cu2-xS) and porphyrin compounds (chlorophyll and chlorophyllin). Fe3O4 and Fe3O4@Cu2-xS are synthesized using various solution methods that produce mono-dispersed nanoparticles on the order of 10 nm. Chlorophyll is extracted from fresh spinach and chlorophyllin sodium copper is a commercial product. These photothermal (PT) materials are dispersed in polymethyl methacrylate (PMMA) solutions and deposited on glass substrates via spin coating that result in clear and transparent thin films. The iron-oxide based thin films show distinctive absorption spectra; Fe3O4 exhibits a strong peak near UV and gradually decreases into the visible and NIR regions; the absorption of Fe3O4@Cu2-xS is similar in the UV region but shows a broad absorption in the NIR region. Both chlorophyll and chlorophyllin are characterized with absorption peaks near UV and NIR showing a “U”-shaped spectrum, ideally required for efficient solar harvest and high transparency in energy-efficient single-pane window applications. Upon coating of the transparent PT films on the window inner surfaces, solar irradiation induces the photothermal effect, consequently raising the film temperature. In this fashion, the thermal loss through the window can be significantly lowered by reducing the temperature difference between the window inner surface and the room interior, based on a new concept of so-called “optical thermal insulation” (OTI) without any intervention medium, such as air/argon, as required in the glazing technologies. Single-panes are therefore possible to replace double- or triple panes. As OTI is inevitably affected by seasonal and daily sunlight changes, an incident light angle dependence of the photothermal effect is crucial in both thin film and window designs. It is found that the heating curves reach their maxima at small angles of incidence while the photothermal effect is considerably reduced at large angles. This angle dependence is well explained by light reflection by the thin film surface, however, deviated from what is predicted by the Fresnel’s law, attributable to non-ideal surfaces of the substrates. The angle dependence data provides an important reference for OTI that window exposure to sun is greater at winter solstice while that is considerably reduced in the summer. This conclusion indicates much enhanced solar harvesting and heat conversion via optically insulated windows in the winter season, resulting in much lower U-factors. 

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2. Effective reduction of building heat loss without insulation materials via the photothermal effect of a chlorophyll thin film coated “Green Window”

   https://doi.org/10.1557/mrc.2019.52  

   Zhao, Yuan; Dunn, Andrew W.; Shi, Donglu (June 2019, MRS Communications)

   One of the critical components of energy savings in buildings is thermal insulation, especially for windows in cold climates. The conventional approach mainly relies on a double-pane design. In this study, a new concept of “Green Window” has been designed for single-pane applications that lower the U-factor. The “Green Window” is structurally and simply composed of a thin film window coating of chlorophyll that exhibits pronounced photothermal effect, while remaining highly transparent. We demonstrate a new concept in “thermal insulation” via optical means instead of solely through thermal insulators or spectral selectivity. This concept lifts the dependence on insulating materials making single-pane window highly possible. 

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3. Pt ₁ –O ₄ as active sites boosting CO oxidation via a non-classical Mars–van Krevelen mechanism

   https://doi.org/10.1039/D1CY00115A  

   Lou, Yang; Zheng, Yongping; Guo, Wenyi; Liu, Jingyue (May 2021, Catalysis Science & Technology)

   null (Ed.)

   Single-atom catalysts (SACs) exhibit excellent performance for various catalytic reactions but it is still challenging to have adequate total activity for practical applications. Here we report the high-valence, square planar Pt 1 –O 4 as an active site that enables significantly to increase the total activity of the Pt 1 /Fe 2 O 3 SAC with a Pt loading of only ∼30 ppm, which is similar to that of a 1.0 wt% nano-Pt/Fe 2 O 3 , for CO oxidation at 350 °C. Density functional theory calculations reveal that Pt 1 –O 4 catalyzes CO oxidation through a non-classical Mars–van Krevelen mechanism. The adsorbed O 2 on Pt 1 atoms activates the coordination oxygen in the Pt 1 –O 4 configuration, and then a barrierless O 2 dissociation occurs on the Pt 1 –Fe 2 triangle to replenish the consumed coordination oxygen by the cooperative action of Pt 5d and Fe 3d electrons. This work provides a new fundamental understanding of oxidation catalysis on stable and active SACs, providing guidance for rationally designing future heterogeneous catalysts. 

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4. Syngas production at a near-unity H ₂ /CO ratio from photo-thermo-chemical dry reforming of methane on a Pt decorated Al ₂ O ₃ –CeO ₂ catalyst

   https://doi.org/10.1039/D1TA10088B  

   Feng, Xuhui; Du, Zichen; Sarnello, Erik; Deng, Wei; Petru, Cullen R.; Fang, Lingzhe; Li, Tao; Li, Ying (April 2022, Journal of Materials Chemistry A)

   In this work, a Pt catalyst supported on an equimolar Al 2 O 3 –CeO 2 binary oxide (Pt–Al–Ce) was prepared and applied in photo-thermo-chemical dry reforming of methane (DRM) driven by concentrated solar irradiation. It was found that the Pt–Al–Ce catalyst showed good stability in DRM reactions and significant enhancements in H 2 and CO production rates compared with Pt/CeO 2 (Pt–Ce) and Pt/Al 2 O 3 (Pt–Al) catalysts. At a reaction temperature of 700 °C under 30-sun equivalent solar irradiation, the Pt–Al–Ce catalyst exhibits a stable DRM catalytic performance at a H 2 production rate of 657 mmol g −1 h −1 and a CO production rate of 666 mmol g −1 h −1 , with the H 2 /CO ratio almost equal to unity. These production rates and the H 2 /CO ratio were significantly higher than those obtained in the dark at the same temperature. The light irradiation was found to induce photocatalytic activities on Pt–Al–Ce and reduce the reaction activation energy. In situ diffuse reflectance infrared Fourier transform spectroscopy ( in situ DRIFTS) was applied to identify the active intermediates in the photo-thermo-chemical DRM process, which were bidentate/monodentate carbonate, absorbed CO on Pt, and formate. The benefits of the binary Al 2 O 3 –CeO 2 substrate could be ascribed to Al 2 O 3 promoting methane dissociation while CeO 2 stabilized and eliminated possible coke formation, leading to high catalytic DRM activity and stability. 

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5. Fe‐Ion Bolted VOPO ₄ ∙2H ₂ O as an Aqueous Fe‐Ion Battery Electrode

   https://doi.org/10.1002/adma.202105234  

   Xu, Yunkai; Wu, Xianyong; Sandstrom, Sean_K; Hong, Jessica_J; Jiang, Heng; Chen, Xin; Ji, Xiulei (October 2021, Advanced Materials)

   Abstract Iron ion batteries using Fe²⁺as a charge carrier have yet to be widely explored, and they lack high‐performing Fe²⁺hosting cathode materials to couple with the iron metal anode. Here, it is demonstrated that VOPO₄∙2H₂O can reversibly host Fe²⁺with a high specific capacity of 100 mAh g⁻¹and stable cycling performance, where 68% of the initial capacity is retained over 800 cycles. In sharp contrast, VOPO₄∙2H₂O's capacity of hosting Zn²⁺fades precipitously over tens of cycles. VOPO₄∙2H₂O stores Fe²⁺with a unique mechanism, where upon contacting the electrolyte by the VOPO₄∙2H₂O electrode, Fe²⁺ions from the electrolyte get oxidized to Fe³⁺ions that are inserted and trapped in the VOPO₄∙2H₂O structure in an electroless redox reaction. The trapped Fe³⁺ions, thus, bolt the layered structure of VOPO₄∙2H₂O, which prevents it from dissolution into the electrolyte during (de)insertion of Fe²⁺. The findings offer a new strategy to use a redox‐active ion charge carrier to stabilize the layered electrode materials. 

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