| 1. |
- Chai, Zhigang
(författare)
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Light-Driven Alcohol Splitting by Heterogeneous Photocatalysis : Recent Advances, Mechanism and Prospects
- 2021
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Ingår i: Chemistry - An Asian Journal. - : John Wiley & Sons. - 1861-4728 .- 1861-471X. ; 16:5, s. 460-473
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Forskningsöversikt (refereegranskat)abstract
- Splitting of alcohols into hydrogen and corresponding carbonyl compounds, also called acceptorless alcohol dehydrogenation, is of great significance for both synthetic chemistry and hydrogen production. Light-Driven Alcohol Splitting (LDAS) by heterogeneous photocatalysis is a promising route to achieve such transformations, and it possesses advantages including high selectivity of the carbonyl compounds, extremely mild reaction conditions (room temperature and irradiation of visible light) and easy separation of the photocatalysts from the reaction mixtures. Because a variety of alcohols can be derived from biomass, LDAS can also be regarded as one of the most sustainable approaches for hydrogen production. In this Review, recent advances in the LDAS catalyzed by the heterogeneous photocatalysts are summarized, focusing on the mechanistic insights for the LDAS and aspects that influence the performance of the photocatalysts from viewpoints of metallic co-catalysts, semiconductors, and metal/semiconductor interfaces. In addition, challenges and prospects have been discussed in order to present a complete picture of this field.
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| 2. |
- Chai, Zhigang, et al.
(författare)
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Ni–Ag Nanostructure-Modified Graphitic Carbon Nitride for Enhanced Performance of Solar-Driven Hydrogen Production from Ethanol
- 2020
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Ingår i: ACS Applied Energy Materials. - : American Chemical Society (ACS). - 2574-0962. ; 3:10, s. 10131-10138
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Tidskriftsartikel (refereegranskat)abstract
- Solar-driven splitting of alcohol utilizing photocatalysts is a promising route to obtain H2 and fine chemicals. Ni nanoparticles have shown great potential for light-driven splitting of alcohol, and their size, exposed facets, and electronic properties play key roles in the performance of photocatalysts. Therefore, purposefully modifying Ni is of great importance. In this report, Ni–Ag nanostructures were fabricated in situ on graphitic carbon nitride by a sequential photodeposition method. The solar-driven hydrogen production from ethanol was dramatically enhanced on the Ni–Ag nanostructure-modified graphitic carbon nitride compared with pure Ni nanoparticle-modified graphitic carbon nitride. It was found that the beneficial role of Ag is to disperse and stabilize small Ni nanoparticles and, importantly, expose catalytic sites that are less prone to accumulate ethanol decomposition products (acetate species), as proven by in situ diffuse reflectance infrared Fourier transform spectroscopy.
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| 3. |
- Hu, Ya, et al.
(författare)
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Autogenic electrolysis of water powered by solar and mechanical energy
- 2022
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Ingår i: Nano Energy. - : Elsevier. - 2211-2855 .- 2211-3282. ; 91
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Tidskriftsartikel (refereegranskat)abstract
- A dual-bandgap photoelectrochemical (PEC) cell with two semiconductors stacked in tandem is a widely adopted concept to capture a large fraction of the solar spectrum for water splitting. While two photons are theoretically needed to produce one H2 molecule using single-bandgap PEC cells, four photons are generally required for one H2 molecule in the dual-bandgap cells because of an unavoidable charge recombination at the solid-solid interface. Here, triboelectric effects are exploited in the form of triboelectric nanogenerator (TENG) to allow for the generation of one H2 molecule at the expenses of two photons in a dual-bandgap device using an array of core/shell p-type silicon/anatase-TiO2 nanowires as photoelectrode. The TENG, that converts mechanical energy to electricity, efficiently suppresses the charge recombination at the interface and significantly increases the energy of the photo-generated carriers required for the simultaneous water reduction and oxidation. The synergy of photoexcitation and triboelectrics results in a rate of hydrogen production in a neutral Na2SO4 electrolyte around 150 times higher than that of the counterpart, i.e., the device in the absence of TENG. Furthermore, the TENG-induced enhancement in the PEC water splitting remains substantial even when the solar power density is reduced to 20 mW/cm2.
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| 4. |
- Klionsky, Daniel J., et al.
(författare)
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Guidelines for the use and interpretation of assays for monitoring autophagy
- 2012
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Ingår i: Autophagy. - : Informa UK Limited. - 1554-8635 .- 1554-8627. ; 8:4, s. 445-544
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Forskningsöversikt (refereegranskat)abstract
- In 2008 we published the first set of guidelines for standardizing research in autophagy. Since then, research on this topic has continued to accelerate, and many new scientists have entered the field. Our knowledge base and relevant new technologies have also been expanding. Accordingly, it is important to update these guidelines for monitoring autophagy in different organisms. Various reviews have described the range of assays that have been used for this purpose. Nevertheless, there continues to be confusion regarding acceptable methods to measure autophagy, especially in multicellular eukaryotes. A key point that needs to be emphasized is that there is a difference between measurements that monitor the numbers or volume of autophagic elements (e.g., autophagosomes or autolysosomes) at any stage of the autophagic process vs. those that measure flux through the autophagy pathway (i.e., the complete process); thus, a block in macroautophagy that results in autophagosome accumulation needs to be differentiated from stimuli that result in increased autophagic activity, defined as increased autophagy induction coupled with increased delivery to, and degradation within, lysosomes (in most higher eukaryotes and some protists such as Dictyostelium) or the vacuole (in plants and fungi). In other words, it is especially important that investigators new to the field understand that the appearance of more autophagosomes does not necessarily equate with more autophagy. In fact, in many cases, autophagosomes accumulate because of a block in trafficking to lysosomes without a concomitant change in autophagosome biogenesis, whereas an increase in autolysosomes may reflect a reduction in degradative activity. Here, we present a set of guidelines for the selection and interpretation of methods for use by investigators who aim to examine macroautophagy and related processes, as well as for reviewers who need to provide realistic and reasonable critiques of papers that are focused on these processes. These guidelines are not meant to be a formulaic set of rules, because the appropriate assays depend in part on the question being asked and the system being used. In addition, we emphasize that no individual assay is guaranteed to be the most appropriate one in every situation, and we strongly recommend the use of multiple assays to monitor autophagy. In these guidelines, we consider these various methods of assessing autophagy and what information can, or cannot, be obtained from them. Finally, by discussing the merits and limits of particular autophagy assays, we hope to encourage technical innovation in the field.
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| 5. |
- Li, Shaowen, et al.
(författare)
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A Multiscale, Dynamic Elucidation of Li Solubility in the Alloy and Metallic Plating Process
- 2023
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Ingår i: Advanced Materials. - : Wiley-VCH Verlagsgesellschaft. - 0935-9648 .- 1521-4095. ; 35:47
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Tidskriftsartikel (refereegranskat)abstract
- Li-containing alloys and metallic deposits offer substantial Li+ storage capacities as alternative anodes to commercial graphite. However, the thermodynamically in sequence, yet kinetically competitive mechanism between Li solubility in the solid solution and intermediate alloy-induced Li deposition remains debated, particularly across the multiple scales. The elucidation of the mechanism is rather challenging due to the dynamic alloy evolution upon the non-equilibrium, transient lithiation processes under coupled physical fields. Here, influential factors governing Li solubility in the Li-Zn alloy are comprehensively investigated as a demonstrative model, spanning from the bulk electrolyte solution to the ion diffusion within the electrode. Through real-time phase tracking and spatial distribution analysis of intermediate alloy/Li metallic species at varied temperatures, current densities and particle sizes, the driving force of Li solubility and metallic plating along the Li migration pathway are probed in-depth. This study investigates the correlation between kinetics (pronounced concentration polarization, miscibility gap in lattice grains) and rate-limiting interfacial charge transfer thermodynamics in dedicating the Li diffusion into the solid solution. Additionally, the lithiophilic alloy sites with the balanced diffusion barrier and Li adsorption energy are explored to favor the homogeneous metal plating, which provides new insights for the rational innovation of high-capacity alloy/metallic anodes.
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| 6. |
- Tesfamhret, Yonas, et al.
(författare)
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On the Manganese Dissolution Process from LiMn2O4 Cathode Materials
- 2021
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Ingår i: ChemElectroChem. - : John Wiley & Sons. - 2196-0216. ; 8:8, s. 1516-1523
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Tidskriftsartikel (refereegranskat)abstract
- Transition metal (TM) dissolution is a process experienced by most cathode materials based on lithium transition metal oxides. Spinel LiMn2O4 (LMO) is the best-known cathode material that suffers from TM dissolution. Therefore, LMO is selected here to understand the dissolution process and derive an inductively coupled plasma optical emission spectroscopy (ICP-OES) method for quantifying dissolved metal ions. Furthermore, the LMO powder is coated with thin Al2O3 films of different thicknesses using atomic layer deposition (ALD) in an attempt to suppress the dissolution of Mn. Two different types of counter electrodes, lithium iron phosphate (LFP) and Li-metal, were used to investigate the role of the counter electrode on Mn dissolution. HF is identified as the lead cause of Mn dissolution, through comparisons of cells containing LiPF6 or LiClO4 based electrolytes. The results show that Li-metal counter electrode effectively minimizes the dissolution process via likely consuming HF and H2O impurity. In contradiction to the purpose of the protective Al2O3 thin film coating, surface coated LMO showed higher dissolution of Mn compared to pristine LMO, both in LFP||LMO and Li||LMO configurations. Al2O3 is proposed to generate H2O when reacts with HF. H2O could have the possibility to migrate back in the electrolyte and participate in the hydrolysis of LiPF6, resulting in more HF and thereby more Mn dissolution.
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| 7. |
- Yang, Chaoran, et al.
(författare)
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Alternate-stacked Li4Ti5O12 nanosheets/d-Ti3C2 flexible film as a current collector-free, high-capacity and robust cathode for rechargeable Mg batteries
- 2020
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Ingår i: Nano select. - : John Wiley & Sons. - 2688-4011. ; 1:1, s. 1-11
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Tidskriftsartikel (refereegranskat)abstract
- Rechargeable magnesium batteries (RMBs) have gained increasing attention owing to its high volumetric capacity, crust abundance, and safety from dendrite-free characteristic. However, the lack of development of high-performance cathode materials with long cycling stability and satisfactory capacity has greatly restricted the development of RMBs. Herein, a self-supported, current collector-free and soft electrode is prepared with delaminated Ti3C2 (d-Ti3C2) and Li4Ti5O12 nanosheets by simple vacuum filtration as flexible cathode in RMBs. Fabricated into a full cell with hybrid AlCl3/MgCl2/Mg(TFSI)2 electrolyte and Mg anode (a thin Mg foil with thickness of 50 μm), the flexible cathode shows high initial specific capacity of 320 mAh g−1 at 20 mA g−1, excellent cycling stability (good retention even after 1000 cycles) and outstanding rate performance. Detailed mechanistic studies reveal that introduction of d-Ti3C2 provide fast transport paths for electrons and Mg2+. The enlarged layer spacing of composited d-Ti3C2 accounts for significant increment in capacity. Benefiting from above-mentioned advantages, the best performance among Ti-based electrode materials is realized and make wearable devices powered by RMBs possible, thus circumventing the safety issues of lithium batteries.
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| 8. |
- Yang, Yuying, et al.
(författare)
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Light-Induced Redox Looping of a Rhodium/CexWO3 Photocatalyst for Highly Active and Robust Dry Reforming of Methane
- 2022
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Ingår i: Angewandte Chemie International Edition. - : John Wiley & Sons. - 1433-7851 .- 1521-3773. ; 61:21
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Tidskriftsartikel (refereegranskat)abstract
- Dry reforming of methane (DRM) has provided an effective avenue to convert two greenhouse gases, CH4 and CO2, into syngas. Here, we design a DRM photocatalyst Rh/CexWO3 that invokes both photothermal and photoelectric processes, which overcomes the thermodynamic limitation of DRM under conventional conditions. In contrast to plasmonic or UV-response photocatalysts, our photocatalyst produces a superior light-to-chemical energy efficiency (LTCEE) of 4.65 % with a moderate light intensity. We propose that a light-induced metal-to-metal charge transfer plays a crucial role in the DRM reaction, which induces a redox looping between Ce to W species to lower the activation energy. Quantum mechanical studies reveal that a high oxygen mobility of CexWO3, accompanied with the formation of oxo-bridge species, results in a substantial elimination of deposited C species during the reaction. Our catalyst design strategy could offer a promising energy-efficient industrial process for DRM.
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