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Non-woven pitch-based carbon fiber electrodes for low-cost redox flow battery† 用于低成本氧化还原液流电池的无纺沥青基碳纤维电极†。
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-15 DOI: 10.1039/D4SE01124D
Abena A. Williams, Sagar V. Kanhere, Amod A. Ogale and Mark E. Roberts

Redox flow batteries (RFBs) are promising energy storage systems to support renewable energy sources and overcome the limitations imposed by their intermittent and unpredictable nature. As a developing technology, the cost of key components, namely the membrane, electrolyte, and electrodes, present a major hurdle to widespread integration. This work describes the performance of non-woven carbon fiber (NWCF) electrodes derived from low-cost petroleum pitch and produced using a scalable, inexpensive melt-blowing process. Compared to commercial polyacrylonitrile (PAN)-based carbon fiber felt, pitch-based carbon fibers have increased graphitic content, tensile strength, and electrical conductivity. Greenhouse gas emissions for pitch-based carbon fibers are estimated to be significantly lower than that of PAN-based carbon fibers. When RFBs with unoptimized NWCF electrodes are evaluated in zinc iodide electrolytes, the voltage and power density (83 mW cm−2) are slightly lower compared to RFBs with PAN-derived carbon felts (104 mW cm−2) @ 100 mA cm−2. RFBs fabricated with oxidized low-cost NWCF electrodes show nearly identical battery performance to those prepared with commercial PAN-derived carbon felts in vanadium electrolytes (peak power density of 137 mW cm−2vs. 139 mW cm−2, respectively). Because of their low-cost precursor and cheaper processing methods, NWCF electrodes offer a promising solution to reducing the cost of RFB electrode materials, and with further optimization, these electrodes will likely result in improved battery performance.

氧化还原液流电池(rfb)是一种很有前途的储能系统,可以支持可再生能源,克服其间歇性和不可预测性所带来的限制。作为一项发展中的技术,膜、电解质和电极等关键部件的成本是广泛集成的主要障碍。这项工作描述了由低成本石油沥青制成的无纺布碳纤维(NWCF)电极的性能,并使用可扩展的、廉价的熔融吹制工艺生产。与商用聚丙烯腈(PAN)基碳纤维毡相比,沥青基碳纤维毡具有更高的石墨含量、抗拉强度和导电性。据估计,沥青基碳纤维的温室气体排放量明显低于pan基碳纤维。当使用未优化的NWCF电极的RFBs在碘化锌电解质中进行评估时,电压和功率密度(83 mW cm - 2)略低于使用pan衍生碳毡的RFBs (104 mW cm - 2) @ 100 mA cm - 2。使用氧化低成本NWCF电极制备的rfb的电池性能与在钒电解质中使用pan衍生碳毡制备的rfb几乎相同(峰值功率密度为137 mW cm - 2vs)。139mw cm−2)。由于其低成本的前驱体和更便宜的加工方法,NWCF电极为降低RFB电极材料的成本提供了一个有前途的解决方案,并且通过进一步优化,这些电极可能会提高电池的性能。
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引用次数: 0
Catechin-induced cellulose: a new material for harvesting triboelectricity 儿茶素诱导的纤维素:一种收获摩擦电的新材料
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-14 DOI: 10.1039/D4SE01443J
P. A. Hisna and P. P. Pradyumnan

The desire to meet energy demands drives us to develop environment-friendly, renewable, and sustainable energy sources. In this study, a catechin (tea dye)-adsorbed cellulose paper-based triboelectric nanogenerator (TAC-TENG) is suggested as an alternative solution. The material employed is tea dust extract incorporated cellulose paper, which are inexpensive, readily available, and eco-friendly. Triboelectric nanogenerator is an electrical energy-harvesting technology, capable of harvesting any kind of low-frequency mechanical energy as an energy source for powering small electronic devices. The proposed TAC-TENG could directly power up 12 white LEDs and store up to 2.08 μJ with a 1 μF capacitor in 80 s. A better performance was displayed by the tea dye-adsorbed cellulose paper than the pristine one. Thus, the proposed TENG could become more relevant and may have a vivid impact in the nearest future. The proposed TAC-TENG could be employed in self-powered portable and wearable small electronic devices.

为满足能源需求,我们致力发展环保、可再生和可持续的能源。在这项研究中,提出了一种吸附儿茶素(茶染料)的纤维素纸基摩擦电纳米发电机(TAC-TENG)作为替代方案。所采用的材料是茶尘提取物结合纤维素纸,价格低廉,易得,环保。摩擦电纳米发电机是一种电能收集技术,能够收集任何一种低频机械能作为小型电子设备供电的能源。所提出的TAC-TENG可以直接为12个白光led供电,并在80s内以1 μF的电容存储高达2.08 μJ的电流。茶染料吸附纤维素纸的性能优于原纸。因此,拟议的TENG可能会变得更加相关,并可能在最近的将来产生生动的影响。提出的TAC-TENG可用于自供电的便携式和可穿戴小型电子设备。
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引用次数: 0
Efficient and stable perovskite solar cells via surface defect passivation using 4-fluorobenzamine trifluoroacetate† 利用4-氟苯扎胺三氟乙酸†通过表面缺陷钝化制备高效稳定的钙钛矿太阳能电池
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-14 DOI: 10.1039/D4SE00473F
Zhongliang Chen, Chao Sun, Hong Wei Qiao, Jiyuan Chen, Xuelu Wang and Yefeng Yao

Perovskite solar cells (PSCs) have achieved high power conversion efficiencies (PCEs). However, surface defects present a major challenge to further improving their performance. Fluorine-substituted materials have been widely utilized to passivate surface defects and improve the photovoltaic performance and stability of PSCs. In this study, post-treatment of the methylamine-lead iodide (MAPbI3) perovskite surface was performed using 4-fluoroaniline trifluoroacetate (P-F-PMATFA), and the surface defects of the perovskite were passivated via an F atom, which reduced the energy barrier between the perovskite film (PVK) and hole transport layer (HTL). Consequently, the PCE of P-F-PMATFA treated solar cells based on the MAPbI3 perovskite increased from 19.19 to 21.01% with low open-circuit voltage (VOC) loss (0.44 V). Further, P-F-PMATFA treated perovskite devices exhibited long-term stability, owing to the higher hydrophobicity of fluorinated materials. The post-treatment strategy demonstrated in this study shows wide application potential in the field of photovoltaic devices owing to its ability to passivate surface defects and improve material stability.

钙钛矿太阳能电池(PSCs)具有很高的功率转换效率(pce)。然而,表面缺陷是进一步提高其性能的主要挑战。氟取代材料已被广泛用于钝化PSCs的表面缺陷,提高其光伏性能和稳定性。本研究采用4-氟苯胺三氟乙酸酯(P-F-PMATFA)对甲基胺-碘化铅(MAPbI3)钙钛矿表面进行后处理,通过F原子钝化钙钛矿表面缺陷,降低钙钛矿膜(PVK)和空穴传输层(HTL)之间的能垒。因此,P-F-PMATFA处理的基于MAPbI3钙钛矿的太阳能电池的PCE从19.19%提高到21.01%,且开路电压(VOC)损失低(0.44 V)。此外,P-F-PMATFA处理的钙钛矿器件由于氟化材料的高疏水性而具有长期稳定性。该后处理策略具有钝化表面缺陷和提高材料稳定性的能力,在光伏器件领域具有广泛的应用潜力。
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引用次数: 0
Kinetic study of catalytic formic acid dehydrogenation by in situ UV-vis spectroscopy†
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-12 DOI: 10.1039/D4SE01328J
Seo Ono, Risheng Li, Chieko Suzuki, Akira Yamamoto, Hisao Yoshida, Hajime Kawanami and Ryoichi Kanega

The development of H2 production technology through formic acid dehydrogenation (FADH), a liquid organic hydrogen carrier, has attracted considerable attention for hydrogen energy utilization. Catalysts play a vital role in FADH. Therefore, it is essential to understand the reaction mechanism and to develop efficient catalysts. Traditionally, theoretical calculations and kinetic isotope effects have been used to analyze the reaction mechanisms; however, achieving accurate kinetic analysis has remained challenging. In response, we devised an analytical method using in situ UV-vis spectroscopy for the kinetic analysis of FADH. The evaluation of the initial hydride formation and H2 evolution rates from dynamic changes observed by in situ UV-vis spectroscopic analysis using a charge coupled device array detector on a millisecond scale suggested the necessity of improving both steps for designing highly active catalysts.

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引用次数: 0
A photo/biocatalytic system for visible-light driven l-alanine production from ammonia and pyruvate† 一个光/生物催化系统,用于可见光驱动氨和丙酮酸生产l-丙氨酸
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-12 DOI: 10.1039/D4SE01215A
Kyosuke Yamada and Yutaka Amao

The chemical structure of L-alanine is similar to that of L-lactic acid and its polymerisation product, poly(L-alanine) (poly-L-Ala), is a biodegradable nylon. There is a need for a method capable of synthesizing L-alanine, a monomer of poly-L-Ala, from a biobased material with a renewable energy source. In this work, visible-light driven L-alanine from biobased material pyruvate and ammonium ions with a system consisting of triethanolamine, water-soluble zinc porphyrin, pentamethylcyclopentadienyl coordinated rhodium complex, NAD+ and L-alanine dehydrogenase from Bacillus subtilis is established. In particular, the conversion yield for pyruvate to L-alanine was improved up to 100% in this system after 24 h irradiation.

l -丙氨酸的化学结构与l -乳酸相似,其聚合产物聚(l -丙氨酸)(聚l -ala)是一种可生物降解的尼龙。需要一种能够用可再生能源从生物基材料合成聚l -ala单体l -丙氨酸的方法。以丙酮酸和铵离子为原料,以三乙乙醇胺、水溶性卟啉锌、五甲基环戊二烯基配位铑配合物、NAD+和枯草芽孢杆菌l -丙氨酸脱氢酶为原料,建立了可见光驱动l -丙氨酸的体系。特别是,在该体系中,经过24 h的辐照,丙酮酸酯转化为l -丙氨酸的收率提高到100%。
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引用次数: 0
Hierarchical ZSM-5 nanosheets for production of light olefins and aromatics by catalytic cracking of oleic acid† 通过催化裂解油酸生产轻烯烃和芳烃的分层 ZSM-5 纳米片†。
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-12 DOI: 10.1039/D4SE01167H
Haoyu Liu, Wenbo Luo, Ke Wang, Yanlin Wang and Hong Yuan

The bolaform surfactant C6H13-N+(CH3)2-C6H12-N+(CH3)2-C6H12-O-C6H4-C6H4-O-C6H12-N+(CH3)2-C6H12-N+(CH3)2-C6H13 (BCPH-6-6-6) was synthesized and used to guide the synthesis of hierarchical ZSM-5 nanosheets (HZN) for use as zeolite catalysts. The number of acidic sites and the Al distribution in the zeolite pores were varied by changing the amounts of sodium sulfate and Al in the initial gel. The X-ray diffraction, Fourier transform infrared spectroscopy, scanning electronic microscopy, NH3 temperature programmed desorption, 27Al magic angle spinning nuclear magnetic resonance spectroscopy and N2 adsorption/desorption were used to characterize these materials. These zeolites each had a well-developed hierarchical system and specific surface areas as high as 631 m2 g−1, indicating that the BCPH-6-6-6 formed lamellar micelles based on π–π stacking. Interconnected hierarchical pore structures were retained after the templating agent was removed. The HZN sample exhibited a 90° rotational intergrowth structure and retained a large number of lamellae. The same material had a high concentration of acidic sites and contained Al in a tetrahedral coordination framework. The catalytic cracking of oleic acid using this zeolite gave light olefin yields up to 52.2% at 500 °C, exceeding the performance of conventional ZSM-5 (38.9%), and the catalyst remained active for up to 60 h. At 450 °C, the BTX selectivity of 6.72% obtained with this material also exceeded that from the conventional ZSM-5. These results were attributed to the connected hierarchical pores of the HZN, which promoted diffusion and provided higher carbon resistance.

合成了波拉形式表面活性剂 C6H13-N+(CH3)2-C6H12-N+(CH3)2-C6H12-O-C6H4-C6H4-O-C6H12-N+(CH3)2-C6H12-N+(CH3)2-C6H13(BCPH-6-6-6),并将其用于指导合成用作沸石催化剂的分层 ZSM-5 纳米片(HZN)。通过改变初始凝胶中硫酸钠和铝的用量,改变了沸石孔隙中酸性位点的数量和铝的分布。利用 X 射线衍射、傅立叶变换红外光谱、扫描电子显微镜、NH3 温编程解吸、27Al 魔角旋转核磁共振波谱和 N2 吸附/解吸来表征这些材料。这些沸石都具有发达的分层体系,比表面积高达 631 m2 g-1,表明 BCPH-6-6 在 π-π 堆积的基础上形成了层状胶束。去除模板剂后,相互连接的分层孔隙结构得以保留。HZN 样品呈现出 90° 旋转互生结构,并保留了大量薄片。同样的材料具有高浓度的酸性位点,并含有四面体配位框架中的铝。使用这种沸石催化油酸裂解,在 500 °C 时轻烯烃产率高达 52.2%,超过了传统 ZSM-5 的性能(38.9%),而且催化剂的活性保持时间长达 60 小时。这些结果归功于 HZN 的连通分层孔隙,它促进了扩散并提供了更高的抗碳性。
{"title":"Hierarchical ZSM-5 nanosheets for production of light olefins and aromatics by catalytic cracking of oleic acid†","authors":"Haoyu Liu, Wenbo Luo, Ke Wang, Yanlin Wang and Hong Yuan","doi":"10.1039/D4SE01167H","DOIUrl":"https://doi.org/10.1039/D4SE01167H","url":null,"abstract":"<p >The bolaform surfactant C<small><sub>6</sub></small>H<small><sub>13</sub></small>-N<small><sup>+</sup></small>(CH<small><sub>3</sub></small>)<small><sub>2</sub></small>-C<small><sub>6</sub></small>H<small><sub>12</sub></small>-N<small><sup>+</sup></small>(CH<small><sub>3</sub></small>)<small><sub>2</sub></small>-C<small><sub>6</sub></small>H<small><sub>12</sub></small>-O-C<small><sub>6</sub></small>H<small><sub>4</sub></small>-C<small><sub>6</sub></small>H<small><sub>4</sub></small>-O-C<small><sub>6</sub></small>H<small><sub>12</sub></small>-N<small><sup>+</sup></small>(CH<small><sub>3</sub></small>)<small><sub>2</sub></small>-C<small><sub>6</sub></small>H<small><sub>12</sub></small>-N<small><sup>+</sup></small>(CH<small><sub>3</sub></small>)<small><sub>2</sub></small>-C<small><sub>6</sub></small>H<small><sub>13</sub></small> (BC<small><sub>PH-6-6-6</sub></small>) was synthesized and used to guide the synthesis of hierarchical ZSM-5 nanosheets (HZN) for use as zeolite catalysts. The number of acidic sites and the Al distribution in the zeolite pores were varied by changing the amounts of sodium sulfate and Al in the initial gel. The X-ray diffraction, Fourier transform infrared spectroscopy, scanning electronic microscopy, NH<small><sub>3</sub></small> temperature programmed desorption, <small><sup>27</sup></small>Al magic angle spinning nuclear magnetic resonance spectroscopy and N<small><sub>2</sub></small> adsorption/desorption were used to characterize these materials. These zeolites each had a well-developed hierarchical system and specific surface areas as high as 631 m<small><sup>2</sup></small> g<small><sup>−1</sup></small>, indicating that the BC<small><sub>PH-6-6-6</sub></small> formed lamellar micelles based on π–π stacking. Interconnected hierarchical pore structures were retained after the templating agent was removed. The HZN sample exhibited a 90° rotational intergrowth structure and retained a large number of lamellae. The same material had a high concentration of acidic sites and contained Al in a tetrahedral coordination framework. The catalytic cracking of oleic acid using this zeolite gave light olefin yields up to 52.2% at 500 °C, exceeding the performance of conventional ZSM-5 (38.9%), and the catalyst remained active for up to 60 h. At 450 °C, the BTX selectivity of 6.72% obtained with this material also exceeded that from the conventional ZSM-5. These results were attributed to the connected hierarchical pores of the HZN, which promoted diffusion and provided higher carbon resistance.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 1","pages":" 152-171"},"PeriodicalIF":5.0,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142844643","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Synergistic effects of liquid phase exfoliated molybdenum based 2D nanosheets and MWCNTs for high performance supercapacitors†
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-12 DOI: 10.1039/D4SE00964A
Riya Malik, Ankur Rana, Megha Rana, Dilip K. Singh, R. Srivastava and C. K. Suman

This work investigates the application of liquid phase exfoliated Mo-based transition metal dichalcogenide (TMDC) two-dimensional (2D) nanosheets integrated with multi-walled carbon nanotubes (MWCNTs) as a novel electrode material for high-performance supercapacitors. The structural, functional, and morphological analyses were performed by XRD, FESEM, XPS, and Raman spectroscopy, which augmented the successful formation of TMDC nanosheets and their nanocomposites with MWCNTs. Structural and morphological characterization studies revealed the successful synthesis of the 2D nanosheets and their intimate integration with the MWCNTs, forming a porous network. Raman spectra confirmed the presence of vibrational bands for TMDC nanosheets (A1g and E2g) and their nanocomposites with MWCNTs (D and G bands). The optical characterisation studies (UV and PL) confirmed the exfoliation of TMDC nanosheets with band gaps of 1.87 eV and 1.67 eV for MoS2 and MoSe2, respectively. From the electrochemical characterisation studies, the values of specific capacitance were found to be 3338.29 F g−1 and 2776.59 F g−1 for MoS2/MWCNT and MoSe2/MWCNT electrodes with energy densities of 102.42 W h kg−1 and 85.18 W h kg−1, respectively. These nanocomposites retained 84% of the initial specific capacitance over 4000 repeated charge/discharge cycles. These nanocomposites may be used as potential materials for the fabrication of next generation devices for energy storage.

{"title":"Synergistic effects of liquid phase exfoliated molybdenum based 2D nanosheets and MWCNTs for high performance supercapacitors†","authors":"Riya Malik, Ankur Rana, Megha Rana, Dilip K. Singh, R. Srivastava and C. K. Suman","doi":"10.1039/D4SE00964A","DOIUrl":"https://doi.org/10.1039/D4SE00964A","url":null,"abstract":"<p >This work investigates the application of liquid phase exfoliated Mo-based transition metal dichalcogenide (TMDC) two-dimensional (2D) nanosheets integrated with multi-walled carbon nanotubes (MWCNTs) as a novel electrode material for high-performance supercapacitors. The structural, functional, and morphological analyses were performed by XRD, FESEM, XPS, and Raman spectroscopy, which augmented the successful formation of TMDC nanosheets and their nanocomposites with MWCNTs. Structural and morphological characterization studies revealed the successful synthesis of the 2D nanosheets and their intimate integration with the MWCNTs, forming a porous network. Raman spectra confirmed the presence of vibrational bands for TMDC nanosheets (A<small><sub>1g</sub></small> and E<small><sub>2g</sub></small>) and their nanocomposites with MWCNTs (D and G bands). The optical characterisation studies (UV and PL) confirmed the exfoliation of TMDC nanosheets with band gaps of 1.87 eV and 1.67 eV for MoS<small><sub>2</sub></small> and MoSe<small><sub>2</sub></small>, respectively. From the electrochemical characterisation studies, the values of specific capacitance were found to be 3338.29 F g<small><sup>−1</sup></small> and 2776.59 F g<small><sup>−1</sup></small> for MoS<small><sub>2</sub></small>/MWCNT and MoSe<small><sub>2</sub></small>/MWCNT electrodes with energy densities of 102.42 W h kg<small><sup>−1</sup></small> and 85.18 W h kg<small><sup>−1</sup></small>, respectively. These nanocomposites retained 84% of the initial specific capacitance over 4000 repeated charge/discharge cycles. These nanocomposites may be used as potential materials for the fabrication of next generation devices for energy storage.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 3","pages":" 750-764"},"PeriodicalIF":5.0,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143107769","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Light-driven water oxidation by a BiVO4/TiO2 photoanode modified with D102 organic dye and copper(ii) meso-tetra(4-carboxyphenyl)porphyrin† 用D102有机染料和铜修饰的BiVO4/TiO2光阳极光驱动水氧化(ii)中四(4-羧基苯基)卟啉†
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-11 DOI: 10.1039/D4SE00543K
Andi Mauliana, Muhammad Iqbal Syauqi, Zico Alaia Akbar, Uji Pratomo, Jacob Yan Mulyana and Tribidasari A. Ivandini

To improve its photoelectrocatalytic water oxidation properties, the BiVO4 photoanode was integrated with TiO2 modified by Indoline D102 dye and copper(II) meso-tetra(4-carboxyphenyl)porphyrin (CuTCPP). The dye was used as a redox mediator, whereas CuTCPP served as a co-catalyst for light-driven water oxidation. The systematic modifications on photoanodes were meticulously characterized by SEM, XRD, UV-Vis spectrometry, and potentiostatic analyses. Modification of the BiVO4 photoanode with TiO2 followed by D102 and CuTCPP (BiVO4/TiO2/D102-CuTCPP) demonstrates a remarkable improvement in photoelectrocatalytic water oxidation properties compared to those of the unmodified BiVO4 film. An increase of power density up to 20 fold was observed under 100 mW cm−2 light irradiation at a bias potential of 1.27 VRHE. The system also demonstrated good stability, with a photocurrent retention of around 97% of the initial photocurrent over a 20 minutes period and retaining 69% of its initial value after 2 hours of continuous operation. Furthermore, the photoelectrocatalytic water splitting exhibited a high faradaic efficiency of oxygen evolution at approximately 97%. These excellent performances were attributed to the synergy of dye and co-catalyst co-assembly by forming a cascade hole transfer mechanism which improves the water oxidation kinetics and reduces the electron–hole recombination rate of BiVO4 in the photoanode system.

为了提高BiVO4光阳极的光电催化水氧化性能,将吲哚啉D102染料修饰的TiO2和铜(II)中四(4-羧基苯基)卟啉(CuTCPP)集成在BiVO4光阳极上。该染料被用作氧化还原介质,而CuTCPP作为光驱动水氧化的助催化剂。通过SEM, XRD, UV-Vis光谱和恒电位分析对光阳极的系统修饰进行了细致的表征。用TiO2修饰BiVO4光阳极,再用D102和CuTCPP修饰BiVO4 (BiVO4/TiO2/D102-CuTCPP),与未修饰的BiVO4膜相比,光电催化水氧化性能显著提高。在偏置电位为1.27 VRHE的100mw cm−2光照射下,观察到功率密度增加了20倍。该系统还显示出良好的稳定性,在20分钟的时间内光电流保持在初始光电流的97%左右,连续工作2小时后保持在初始光电流的69%左右。此外,光电催化水裂解的析氧法拉第效率约为97%。这些优异的性能归因于染料和助催化剂的协同作用,形成了级联空穴转移机制,改善了水氧化动力学,降低了BiVO4在光阳极体系中的电子-空穴复合速率。
{"title":"Light-driven water oxidation by a BiVO4/TiO2 photoanode modified with D102 organic dye and copper(ii) meso-tetra(4-carboxyphenyl)porphyrin†","authors":"Andi Mauliana, Muhammad Iqbal Syauqi, Zico Alaia Akbar, Uji Pratomo, Jacob Yan Mulyana and Tribidasari A. Ivandini","doi":"10.1039/D4SE00543K","DOIUrl":"https://doi.org/10.1039/D4SE00543K","url":null,"abstract":"<p >To improve its photoelectrocatalytic water oxidation properties, the BiVO<small><sub>4</sub></small> photoanode was integrated with TiO<small><sub>2</sub></small> modified by Indoline D102 dye and copper(<small>II</small>) meso-tetra(4-carboxyphenyl)porphyrin (CuTCPP). The dye was used as a redox mediator, whereas CuTCPP served as a co-catalyst for light-driven water oxidation. The systematic modifications on photoanodes were meticulously characterized by SEM, XRD, UV-Vis spectrometry, and potentiostatic analyses. Modification of the BiVO<small><sub>4</sub></small> photoanode with TiO<small><sub>2</sub></small> followed by D102 and CuTCPP (BiVO<small><sub>4</sub></small>/TiO<small><sub>2</sub></small>/D102-CuTCPP) demonstrates a remarkable improvement in photoelectrocatalytic water oxidation properties compared to those of the unmodified BiVO<small><sub>4</sub></small> film. An increase of power density up to 20 fold was observed under 100 mW cm<small><sup>−2</sup></small> light irradiation at a bias potential of 1.27 V<small><sub>RHE</sub></small>. The system also demonstrated good stability, with a photocurrent retention of around 97% of the initial photocurrent over a 20 minutes period and retaining 69% of its initial value after 2 hours of continuous operation. Furthermore, the photoelectrocatalytic water splitting exhibited a high faradaic efficiency of oxygen evolution at approximately 97%. These excellent performances were attributed to the synergy of dye and co-catalyst co-assembly by forming a cascade hole transfer mechanism which improves the water oxidation kinetics and reduces the electron–hole recombination rate of BiVO<small><sub>4</sub></small> in the photoanode system.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 24","pages":" 5927-5936"},"PeriodicalIF":5.0,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142761593","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A fluorine doped carbon aerogel prepared from the spent cathode carbon of aluminum electrolysis towards electrocatalytic synthesis of H2O2† 用铝电解废阴极炭制备含氟碳气凝胶,用于电催化合成H2O2†
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-11 DOI: 10.1039/D4SE01505C
Zhaoxu Li, Yu Liu, Junlang Zhang, Chao Yang, Xintai Su, Chenyuan Zhu, Yongjun Jiang, Wenxin Zhao, Bo Zeng, Chenxi Zhao, Xueli Huang, Hongtao Xie and Yizhao Li

The sustainability of aluminum electrolysis spent cathode carbon (SCC) is currently an urgent environmental issue that needs to be addressed. In this work, fluorine doped carbon aerogels (SCC-FCAs) were prepared by a series of auxiliary purification methods using the graphite phase and fluoride salt phase of SCC in aluminum electrolysis. The obtained SCC-FCAs were used for electrocatalytic synthesis of H2O2 and their performance was evaluated. The experimental results showed that the selectivity of SCC-FCA-500 (heat treatment at 500 °C) reached 87.2%, and the highest yield could reach 900.1 mmol g−1 h−1. The density functional theory calculation results showed that the covalent C–F bond model has weaker adsorption capacity for *OOH than the semi-ionic C–F bond. In addition, the intersite of the semi-ionic C–F in SCC-FCA-500 is the active site for the adsorption of the intermediate *OOH. This work proposed a self-synthesis strategy of using SCC from aluminum electrolysis, which provided a case for the high-value utilization of SCC in the direction of new energy resources.

铝电解废阴极炭(SCC)的可持续性是当前急需解决的环境问题。本文以铝电解中氟掺杂碳的石墨相和氟盐相为原料,采用一系列辅助纯化方法制备了氟掺杂碳气凝胶(SCC- fcas)。将所得的SCC-FCAs用于电催化合成H2O2,并对其性能进行了评价。实验结果表明,SCC-FCA-500(500℃热处理)的选择性达到87.2%,收率最高可达900.1 mmol g−1 h−1。密度泛函理论计算结果表明,共价C-F键模型对*OOH的吸附能力弱于半离子型C-F键。此外,SCC-FCA-500中半离子型C-F的中间位点是中间体*OOH吸附的活性位点。本工作提出了一种利用铝电解SCC的自合成策略,为SCC在新能源方向的高价值利用提供了一个案例。
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引用次数: 0
Technical, environmental and economic analysis of utilizing hydrogen-rich fuel in decarbonized container ships† 脱碳集装箱船使用富氢燃料的技术、环境和经济分析
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-11 DOI: 10.1039/D4SE01109K
Payam Shafie, Alain DeChamplain and Julien Lepine

This paper analyzes the substitution of conventional fuels with hydrogen-rich fuel derived from ammonia for two different types of container ships, focusing on technical, environmental, and economic perspectives. Four operation modes are investigated including marine diesel oil (MDO), dual-fuel (50 : 50 and 25 : 75 percentages of MDO : H2-rich fuel) and pure H2-rich fuel. The environmental impact of using H2-rich fuel is assessed based on the tank-to-wake and well-to-wake CO2-equivalent emissions, considering different ammonia production pathways. The results reveal that all the alternative modes exhibit decreased tank-to-wake emissions compared to MDO. The minimum reduction percentage is related to the 50 : 50 mode at about 44%, and an average well-to-wake reduction of 3.5 and 6.3 g per t NM is achievable by using blue and green ammonia, respectively. Moreover, to avoid any increase in the total costs of alternative modes compared to the reference mode, the future ammonia fuel price should be less than 384 $ per t. The research demonstrates that H2-rich fuel is a viable alternative fuel for container ships, providing notable environmental benefits. While initial costs are higher, long-term economic advantages can be achieved through carbon pricing.

本文从技术、环境和经济的角度分析了两种不同类型的集装箱船用氨衍生的富氢燃料替代传统燃料的情况。研究了船用柴油(MDO)、双燃料(50:50和25:75百分比的MDO:富h2燃料)和纯富h2燃料四种运行模式。考虑到不同的氨生产途径,根据罐到尾流和井到尾流的二氧化碳当量排放来评估使用富h2燃料的环境影响。结果表明,与MDO相比,所有替代模式都表现出减少的罐尾排放。最小减量百分比与50:50模式有关,约为44%,使用蓝色和绿色氨分别可实现3.5和6.3 g / t NM的井尾平均减量。此外,为了避免替代模式与参考模式相比总成本的增加,未来氨燃料的价格应低于384美元/吨。研究表明,富h2燃料是一种可行的集装箱船替代燃料,具有显著的环境效益。虽然初始成本较高,但可以通过碳定价实现长期经济优势。
{"title":"Technical, environmental and economic analysis of utilizing hydrogen-rich fuel in decarbonized container ships†","authors":"Payam Shafie, Alain DeChamplain and Julien Lepine","doi":"10.1039/D4SE01109K","DOIUrl":"https://doi.org/10.1039/D4SE01109K","url":null,"abstract":"<p >This paper analyzes the substitution of conventional fuels with hydrogen-rich fuel derived from ammonia for two different types of container ships, focusing on technical, environmental, and economic perspectives. Four operation modes are investigated including marine diesel oil (MDO), dual-fuel (50 : 50 and 25 : 75 percentages of MDO : H<small><sub>2</sub></small>-rich fuel) and pure H<small><sub>2</sub></small>-rich fuel. The environmental impact of using H<small><sub>2</sub></small>-rich fuel is assessed based on the tank-to-wake and well-to-wake CO<small><sub>2</sub></small>-equivalent emissions, considering different ammonia production pathways. The results reveal that all the alternative modes exhibit decreased tank-to-wake emissions compared to MDO. The minimum reduction percentage is related to the 50 : 50 mode at about 44%, and an average well-to-wake reduction of 3.5 and 6.3 g per t NM is achievable by using blue and green ammonia, respectively. Moreover, to avoid any increase in the total costs of alternative modes compared to the reference mode, the future ammonia fuel price should be less than 384 $ per t. The research demonstrates that H<small><sub>2</sub></small>-rich fuel is a viable alternative fuel for container ships, providing notable environmental benefits. While initial costs are higher, long-term economic advantages can be achieved through carbon pricing.</p>","PeriodicalId":104,"journal":{"name":"Sustainable Energy & Fuels","volume":" 1","pages":" 185-197"},"PeriodicalIF":5.0,"publicationDate":"2024-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142844645","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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Sustainable Energy & Fuels
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