A series of novel CoFe-based catalysts are successfully fabricated by hydrogen reduction of CoFeAl layered-double-hydroxide (LDH) nanosheets at 300-700 °C. The chemical composition and morphology of the reaction products (denoted herein as CoFe-x) are highly dependent on the reduction temperature (x). CO hydrogenation experiments are conducted on the CoFe-x catalysts under UV-vis excitation. With increasing LDH-nanosheet reduction temperature, the CoFe-x catalysts show a progressive selectivity shift from CO to CH , and eventually to high-value hydrocarbons (C ). CoFe-650 shows remarkable selectivity toward hydrocarbons (60% CH , 35% C ). X-ray absorption fine structure, high-resolution transmission electron microscopy, Mössbauer spectroscopy, and density functional theory calculations demonstrate that alumina-supported CoFe-alloy nanoparticles are responsible for the high selectivity of CoFe-650 for C hydrocarbons, also allowing exploitation of photothermal effects. This study demonstrates a vibrant new catalyst platform for harnessing clean, abundant solar-energy to produce valuable chemicals and fuels from CO .
Catalytic C1 chemistry based on the activation/conversion of synthesis gas (CO+H2), methane, carbon dioxide, and methanol offers great potential for the sustainable development of hydrocarbon fuels to replace oil, coal, and natural gas. Traditional thermal catalytic processes used for C1 transformations require high temperatures and pressures, thereby carrying a significant carbon footprint. In comparison, solar‐driven C1 catalysis offers a greener and more sustainable pathway for manufacturing fuels and other commodity chemicals, although conversion efficiencies are currently too low to justify industry investment. In this Review, we highlight recent advances and milestones in light‐driven C1 chemistry, including solar Fischer–Tropsch synthesis, the water‐gas‐shift reaction, CO2 hydrogenation, as well as methane and methanol conversion reactions. Particular emphasis is placed on the rational design of catalysts, structure–reactivity relationships, as well as reaction mechanisms. Strategies for scaling up solar‐driven C1 processes are also discussed.
-Attributed to its advantages of super mechanical flexibility, very low-temperature processing, and compatibility with low cost and high throughput manufacturing, organic thin-film transistor (OTFT) technology is able to bring electrical, mechanical, and industrial benefits to a wide range of new applications by activating nonflat surfaces with flexible displays, sensors, and other electronic functions. Despite both strong application demand and these significant technological advances, there is still a gap to be filled for OTFT technology to be widely commercially adopted. This paper provides a comprehensive review of the current status of OTFT technologies ranging from material, device, process, and integration, to design and system applications, and clarifies the real challenges behind to be addressed.
environmentally friendly energy storage devices. As an emerging energy powering sources, supercapacitors (SCs) hold a vital and individual position owing to their high power density, excellent cycling stability, fast charge/discharge process as well as noticeable reliability, tremendously bridging the gap between rechargeable batteries and traditional capacitors in terms of energy density and power density. [1][2][3][4] Nevertheless, their commercial applications are still seriously impeded since energy densities of SCs are far lagging behind rechargeable batteries. [5,6] In the light of the critical parameters that decide the energy density (E = 1/2CV 2 ) of supercapacitor devices, [7][8][9] substantial efforts have been dedicated to maximizing the energy density via elevating the overall cell voltage (V) and total specific capacitance (C) governed by negative and positive electrodes. Configuration of asymmetric supercapacitors (ASCs) has emerged as a desirable strategy because of the expanded V arised from the absolutely opposite potential window of the two dissimilar electrode materials. [10][11][12] Accordingly, considerable research interest has been invested in constructing highly capacitive negative and positive electrode materials.Until now, transition metal oxides, hydroxides, or phosphides, especially Ni-Co compounds with low cost, natural abundance, and environmentally benign, are mostly employed as positive electrode materials in ASCs because they can present variable oxidation states, favorable electrochemical activity, and large theoretical-specific capacitance based on redox reactions, so they have received extensive attentions as perfect candidates in ASCs. [13][14][15][16][17][18] However, in comparison of the extraordinary advancement obtained by positive electrode materials, the lack of desired negative electrodes restricts the progress of high-performance ASCs. Previously, carbonaceous materials are still the most widely used as negative electrode, giving rise to low-specific capacitance of 100-250 F g −1 . [19][20][21][22][23] In this regard, pseudocapacitive negative electrode materials are proposed to be hopeful alternatives, whereas the restricted studies and poor , even when charging the device within 6.5 s, the energy density can still maintain as high as 45 W h kg −1 at 26.1 kW kg −1 , and the ASC manifests long cycling lifespan with 86.6% capacitance retention even after 5000 cycles. This pioneering work not only offers an attractive strategy for rational construction of high-performance SiC NW-based nanostructured electrodes materials, but also provides a fresh route for manufacturing next-generation high-energy storage and conversion systems.
Small-angle light scattering and ultra small-angle X-ray scattering are used to assess the morphology of single-walled (SWNTs) and multi-walled carbon nanotubes (MWNTs). For MWNTs, a powerlaw scattered-intensity profile with a slope of -1.08 is consistent with the rod-like morphology. For SWNTs, however, scattering profiles characteristic of rod-like morphology are not observed on any length-scale from 1 nm to 50 µm. Rather, disordered objects are found that we identify as a network of carbon "ropes" enmeshed with polyelectrolyte dispersants. The effectiveness of polyelectrolyte dispersants is assessed using small-angle light scattering in conjunction with exposure to ultrasound. In the presence of an anionic polyelectrolyte, sonication can assist dispersion of both SWNTs and MWNTs. In the presence of a cationic agent, however, sonication can induce aggregation. SWNTs respond differently to ultrasound depending on whether residual synthesis catalyst is present. Four dispersants are studied, of which sodium polystyrene sulfonate is the most effective and polyallylamine hydrochloride is the least effective.
Conversion of syngas (CO, H ) to hydrocarbons, commonly known as the Fischer-Tropsch (FT) synthesis, represents a fundamental pillar in today's chemical industry and is typically carried out under technically demanding conditions (1-3 MPa, 300-400 °C). Photocatalysis using sunlight offers an alternative and potentially more sustainable approach for the transformation of small molecules (H O, CO, CO , N , etc.) to high-valuable products, including hydrocarbons. Herein, a novel series of Fe-based heterostructured photocatalysts (Fe-x) is successfully fabricated via H reduction of ZnFeAl-layered double hydroxide (LDH) nanosheets at temperatures (x) in the range 300-650 °C. At a reduction temperature of 500 °C, the heterostructured photocatalyst formed (Fe-500) consists of Fe and FeO nanoparticles supported by ZnO and amorphous Al O . Fe-500 demonstrates remarkable CO hydrogenation performance with very high initial selectivities toward hydrocarbons (89%) and especially light olefins (42%), and a very low selectivity towards CO (11%). The intimate and abundant interfacial contacts between metallic Fe and FeO in the Fe-500 photocatalyst underpins its outstanding photocatalytic performance. The photocatalytic production of high-value light olefins with suppressed CO selectivity from CO hydrogenation is demonstrated here.
Photocatalysis as one of the future environment technologies has been investigated for decades.D espite great efforts in catalyst engineering,t he widely used powder dispersion and photoelectrode systems are still restricted by sluggish interfacial mass transfer and chemical processes.Here we develop ascalable bilayer paper from commercialized TiO 2 and carbon nanomaterials,s elf-supported at gas-liquid-solid interfaces for photothermal-assisted triphase photocatalysis. The photogeneration of reactive oxygen species can be facilitated through fast oxygen diffusion over triphase interfaces,w hile the interfacial photothermal effect promotes the following free radical reaction for advanced oxidation of phenol. Under full spectrum irradiation, the triphase system shows 13 times higher reaction rate than diphase controlled system, achieving 88.4 %mineralization of high concentration phenol within 90 min full spectrum irradiation. The bilayer paper also exhibits high stability over 40 times cycling experiments and sunlight driven feasibility,s howing potentials for large scale photocatalytic applications by being further integrated into atriphase flowr eactor.
Methane conversion to higher hydrocarbons requires harsh reaction conditions due to high energy barriers associated with CÀ H bond activation. Herein, we report a systematic investigation of photocatalytic oxidative coupling of methane (OCM) over transitionmetal-loaded ZnO photocatalysts. A 1 wt % Au/ZnO delivered a remarkable C 2 -C 4 hydrocarbon production rate of 683 μmol g À 1 h À 1 (83 % C 2 -C 4 selectivity) under light irradiation with excellent photostability over two days. The metal type and its interaction with ZnO strongly influence the selectivity toward CÀ C coupling products. Photogenerated Zn + -O À sites enable CH 4 activation to methyl intermediates (*CH 3 ) migrating onto adjacent metal nanoparticles. The nature of the *CH 3 -metal interaction controls the OCM products. In the case of Au, strong d-σ orbital hybridization reduces metal-CÀ H bond angles and steric hindrance, thereby enabling efficient methyl coupling. Findings indicate the d-σ center may be a suitable descriptor for predicting product selectivity during OCM over metal/ZnO photocatalysts.
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