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      Photoelectrochemical reduction of N 2 to NH 3 under ambient conditions through hierarchical MoSe 2@g-C 3N 4 heterojunctions

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          Abstract

          Ammonia is the main precursor for the production of fertilizers, a hydrogen energy carrier and an emerging clean fuel that plays a crucial role in sustaining life on the globe.

          Abstract

          Ammonia is the main precursor for the production of fertilizers, a hydrogen energy carrier and an emerging clean fuel that plays a crucial role in sustaining life on the globe. Herein, hybrid MoSe 2@g-C 3N 4 micro/nanostructures are described that can serve as photoelectrochemical (PEC) catalysts to fix N 2 into NH 3 in a basic electrolyte at a low potential (−0.3 V vs. RHE) under ambient conditions. In situ functionalization of the hierarchical micro/nanoflowers of MoSe 2 with exfoliated g-C 3N 4 nanosheets dramatically boosts the faradaic efficiency and yield rate up to 28.91% and 7.72 μmol h −1 cm −2 respectively. The high PEC activity can be attributed to the hierarchical architecture, light-harvesting capability, tunable active sites and formation of heterojunctions, as confirmed by various characterization and density functional theory (DFT) calculations. Therefore, this work not only develops an effective procedure to obtain hierarchical heterojunction catalysts towards a high-efficiency NRR but also provides a deep understanding of artificial N 2 fixation at the MoSe 2@g-C 3N 4 interface.

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          Structural absorption by barbule microstructures of super black bird of paradise feathers

          Dakota E. McCoy, Teresa J. Feo, Todd Alan Harvey … (2018)
          Many studies have shown how pigments and internal nanostructures generate color in nature. External surface structures can also influence appearance, such as by causing multiple scattering of light (structural absorption) to produce a velvety, super black appearance. Here we show that feathers from five species of birds of paradise (Aves: Paradisaeidae) structurally absorb incident light to produce extremely low-reflectance, super black plumages. Directional reflectance of these feathers (0.05–0.31%) approaches that of man-made ultra-absorbent materials. SEM, nano-CT, and ray-tracing simulations show that super black feathers have titled arrays of highly modified barbules, which cause more multiple scattering, resulting in more structural absorption, than normal black feathers. Super black feathers have an extreme directional reflectance bias and appear darkest when viewed from the distal direction. We hypothesize that structurally absorbing, super black plumage evolved through sensory bias to enhance the perceived brilliance of adjacent color patches during courtship display.
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            Graphitic Carbon Nitride (g-C3N4)-Based Photocatalysts for Artificial Photosynthesis and Environmental Remediation: Are We a Step Closer To Achieving Sustainability?

            Wee-Jun Ong, Lling-Lling Tan, Yun Ng … (2016)
            As a fascinating conjugated polymer, graphitic carbon nitride (g-C3N4) has become a new research hotspot and drawn broad interdisciplinary attention as a metal-free and visible-light-responsive photocatalyst in the arena of solar energy conversion and environmental remediation. This is due to its appealing electronic band structure, high physicochemical stability, and "earth-abundant" nature. This critical review summarizes a panorama of the latest progress related to the design and construction of pristine g-C3N4 and g-C3N4-based nanocomposites, including (1) nanoarchitecture design of bare g-C3N4, such as hard and soft templating approaches, supramolecular preorganization assembly, exfoliation, and template-free synthesis routes, (2) functionalization of g-C3N4 at an atomic level (elemental doping) and molecular level (copolymerization), and (3) modification of g-C3N4 with well-matched energy levels of another semiconductor or a metal as a cocatalyst to form heterojunction nanostructures. The construction and characteristics of each classification of the heterojunction system will be critically reviewed, namely metal-g-C3N4, semiconductor-g-C3N4, isotype g-C3N4/g-C3N4, graphitic carbon-g-C3N4, conducting polymer-g-C3N4, sensitizer-g-C3N4, and multicomponent heterojunctions. The band structures, electronic properties, optical absorption, and interfacial charge transfer of g-C3N4-based heterostructured nanohybrids will also be theoretically discussed based on the first-principles density functional theory (DFT) calculations to provide insightful outlooks on the charge carrier dynamics. Apart from that, the advancement of the versatile photoredox applications toward artificial photosynthesis (water splitting and photofixation of CO2), environmental decontamination, and bacteria disinfection will be presented in detail. Last but not least, this comprehensive review will conclude with a summary and some invigorating perspectives on the challenges and future directions at the forefront of this research platform. It is anticipated that this review can stimulate a new research doorway to facilitate the next generation of g-C3N4-based photocatalysts with ameliorated performances by harnessing the outstanding structural, electronic, and optical properties for the development of a sustainable future without environmental detriment.
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              Rational design of electrocatalysts and photo(electro)catalysts for nitrogen reduction to ammonia (NH3) under ambient conditions

              Shi-Zhang Qiao, Chunxian Guo, Jingrun Ran … (2018)
              This perspective highlights the rational design of efficient electrocatalysts and photo(electro)catalysts for N 2 reduction to ammonia (NH 3 ) under ambient conditions. As one of the most important chemicals and carbon-free energy carriers, ammonia (NH 3 ) has a worldwide annual production of ∼150 million tons, and is mainly produced by the traditional high-temperature and high-pressure Haber–Bosch process which consumes massive amounts of energy. Very recently, electrocatalytic and photo(electro)catalytic reduction of N 2 to NH 3 , which can be performed at ambient conditions using renewable energy, have received tremendous attention. The overall performance of these electrocatalytic and photo(electro)catalytic systems is largely dictated by their core components, catalysts. This perspective for the first time highlights the rational design of electrocatalysts and photo(electro)catalysts for N 2 reduction to NH 3 under ambient conditions. Fundamental theory of catalytic reaction pathways for the N 2 reduction reaction and the corresponding material design principles are introduced first. Then, recently developed electrocatalysts and photo(electro)catalysts are summarized, with a special emphasis on the relationship between their physicochemical properties and NH 3 production performance. Finally, the opportunities in this emerging research field, in particular, the strategy of combining experimental and theoretical techniques to design efficient and stable catalysts for NH 3 production, are outlined.
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                Author and article information

                Contributors
                Journal
                Journal ID (publisher-id): JMCAET
                Title: Journal of Materials Chemistry A
                Abbreviated Title: J. Mater. Chem. A
                Publisher: Royal Society of Chemistry (RSC)
                ISSN (Print): 2050-7488
                ISSN (Electronic): 2050-7496
                Publication date Created: February 9 2021
                Publication date (Electronic): 2021
                Volume: 9
                Issue: 5
                Pages: 2742-2753
                Affiliations
                [1 ]State Key Laboratory of Chemical Resource Engineering
                [2 ]Beijing University of Chemical Technology
                [3 ]Beijing 100029
                [4 ]People's Republic of China
                [5 ]Beijing Key Laboratory of Energy Conversion and Storage Materials
                [6 ]College of Chemistry
                [7 ]Beijing Normal University
                [8 ]Beijing 100875
                Article
                DOI: 10.1039/D0TA10620H
                SO-VID: 8e946f2c-d150-4080-8cac-9c79317a5d1e
                Copyright © © 2021
                License:

                http://rsc.li/journals-terms-of-use

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