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Ag–NiP deposited green carbon channel embedded NiP panels for sustainable water splitting† 用于可持续水分离的 Ag-NiP 沉积绿色碳通道嵌入式 NiP 面板
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-09-12 DOI: 10.1039/D4YA00463A
Revathy B. Nair, A. Anantha Krishnan, Aneesh Kumar M. A., Sivaraj Rajendran, Sreehari Harikumar, Vidhya C., M. Ameen Sha, Thomas Mathew, Sajith Kurian and P. S. Arun

Ag–NiP-deposited carbon channels on NiP panels were successfully developed through lemon juice extract (Ag–CL/NiP) and citric acid (Ag–CC/NiP)-assisted methodologies. The methods involved the precise execution of electroless deposition of the advanced Ag–carbon matrix with NiP. The lemon juice-assisted method produced carbon channels with a dense concentration of Ag–NiP on the electrode surface, whereas the citric acid method resulted in a less dense deposition of Ag–NiP on the electrode surface, as observed via FE-SEM. The Ag–CL/NiP has remarkably higher electro- and photocatalytic water splitting performance due to the compact and conductive Ag–NiP connected with carbon channels. Electrochemical impedance analysis of Ag–CL/NiP revealed a low Rct of 491.3 Ω at the open circuit potential, indicating enhanced conductivity. The electrocatalytic oxygen evolution reaction (OER) overpotential of Ag–CL/NiP was 401 mV to achieve a current density of 50 mA cm−2, with a Tafel slope of 46.5 mV dec−1. The panel exhibited good stability, with a proven durability of over 1000 cycles of CV during OER. The developed panel achieved an impressive photocurrent density of ∼9.5 mA cm−2 at 1.37 V vs. RHE when subjected to light irradiation with a wavelength exceeding 420 nm. Furthermore, the Ag–CL/NiP panel demonstrated the ability to generate 17.5 mmol cm−2 of H2 over a 4-hour sunlight irradiation period. The temperature-controlled photocatalytic water splitting experiment revealed that the panel maintained its activity at temperatures as low as ∼12 °C, but with a 40% drop in efficiency compared to normal sunlight conditions.

通过柠檬汁提取物(Ag-CL/NiP)和柠檬酸(Ag-CC/NiP)辅助方法,成功地在 NiP 面板上开发了 Ag-NiP 沉积碳通道。这两种方法都是将先进的银碳基质与 NiP 一起进行精确的无电解沉积。根据 FE-SEM 的观察,柠檬汁辅助法在电极表面生成了 Ag-NiP 浓度较高的碳通道,而柠檬酸法在电极表面沉积的 Ag-NiP 浓度较低。Ag-CL/NiP 的电化学阻抗分析表明,在开路电位下,Ag-CL/NiP 的 Rct 低至 491.3 Ω,表明其导电性能得到了增强。Ag-CL/NiP 的电催化氧进化反应(OER)过电位为 401 mV,电流密度为 50 mA cm-2,塔菲尔斜率为 46.5 mV.dec-1。该面板显示出良好的稳定性,在 OER 期间的 CV 耐久性超过 1000 次。当受到波长超过 420 nm 的光照射时,所开发的面板在 1.37 V 对比 RHE 时达到了令人印象深刻的 9.5 mA cm-² 光电流密度。此外,Ag-CL/NiP 面板在 4 小时的日光照射期间能够产生 17.5 mmol cm-² 的 H₂。温控光催化水分离性能表明,该面板在 12°C 以下的低温条件下仍能保持活性,但光催化效率比正常日照条件下降低了 40%。
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引用次数: 0
Electrochemical and spectroscopic characterisation of organic molecules with high positive redox potentials for energy storage in aqueous flow cells† 用于水流电池储能的高正氧化还原电位有机分子的电化学和光谱特性分析
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-09-11 DOI: 10.1039/D4YA00366G
Christopher G. Cannon, Peter A. A. Klusener, Nigel P. Brandon and Anthony R. J. Kucernak

We show that a number of ubiquitous organic molecules used as redox mediators and chemically sensing species can be used as positive couples in electrochemical energy storage. Air and acid stable organic molecules were tested in aqueous acid electrolytes and employed as the positive electrolyte in H2–organic electrochemical cells. The dissolved organic species were characterised in-operando using UV-vis spectroscopy. N,N,N,N′-tetramethylbenzidine was found to be a stable and reversible redox organic molecule, with a 2 e molecule−1 capacity and a 0.83 V cell potential. N-Oxyl species were also tested in purely aqueous acidic flow battery electrolytes. A H2–violuric acid cell produced a reversible potential of 1.16 V and demonstrated promising redox flow cell cycling performance.

我们的研究表明,一些用作氧化还原介质和化学传感物种的无处不在的有机分子可用作电化学储能中的正偶联剂。我们在酸性水电解质中测试了空气和酸性稳定的有机分子,并将其用作 H2- 有机电化学电池中的正电解质。使用紫外-可见光谱对溶解的有机物进行了表征。结果发现,N,N,N′,N′-四甲基联苯胺是一种稳定的可逆氧化还原有机分子,电容量为 2 e- molecule-1,电池电位为 0.83 V。还在纯水性酸性液流电池电解质中测试了 N-氧物种。H2--violuric 酸电池产生了 1.16 V 的可逆电位,显示了氧化还原流动电池循环性能的良好前景。
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引用次数: 0
Tautomerism and nucleophilic addition influence the performance of aqueous organic redox flow batteries of chelidamic acid and chelidonic acid† 同分异构和亲核加成影响螯合氨基甲酸和螯合酮酸水有机氧化还原流电池的性能
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-09-05 DOI: 10.1039/D4YA00331D
Surya Prakash, Alagar Ramar, Fu-Ming Wang, Kefyalew Wagari Guji, Citra Deliana Dewi Sundari and Laurien Merinda

The redox flow battery is a cost-effective solution for grid-scale energy storage. Its special feature of separate reservoirs and electrodes makes it easy to adjust the electrolyte volume and electrode size, improving safety and scalability. In this work, we explore two organic anolytes, chelidamic acid (CDA) and chelidonic acid (CDO), which share similar molecular weight but differ in their heteroatoms: pyridone and pyrone. The half-cell potentials of the CDA and CDO anolytes enable them to exhibit theoretical cell voltages of 0.49 V and 0.48 V, respectively, when coupled with K4[FeII(CN)6] catholyte. CDA demonstrated a stable discharge capacity of 650 mA h L−1 over 17 days in a basic medium without any degradation. In contrast, CDO gradually loses its capacity over successive cycles. The mechanism for the decomposition of CDO was analysed through cyclic voltammetry, 1H-NMR, and FTIR spectroscopy techniques. The analytical results revealed that there was a significant impact of tautomerization in CDA and nucleophilic addition in CDO on the performance in ARFBs.

氧化还原液流电池是一种经济高效的电网级储能解决方案。氧化还原液流电池具有储液器和电极分离的特点,易于调节电解质体积和电极尺寸,从而提高了安全性和可扩展性。在这项研究中,我们探讨了两种有机鳌合物:螯合氨基甲酸(CDA)和螯合onic酸(CDO),它们具有相似的分子量,但在杂原子上存在差异:吡啶酮和吡喃酮。当与 K_4 [Fe^II (CN)_6] 电解质结合使用时,CDA 和 CDO 的半电池电位使它们的理论电池电压分别达到 0.49 V 和 0.48 V。CDA 在碱性介质中稳定放电 17 天,放电容量达 650 mAh/L,且无任何降解。与此相反,CDO 在连续循环中逐渐失去容量。我们通过循环伏安法、1H-NMR 和傅立叶变换红外光谱技术分析了 CDO 的分解机理。分析结果表明,CDA 中的同分异构和 CDO 中的亲核加成对 ARFB 的性能有显著影响。
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引用次数: 0
Multi-metal (Fe, Cu, and Zn) coordinated hollow porous dodecahedron nanocage catalyst for oxygen reduction in Zn–air batteries† 多金属(铁、铜、锌)配位空心多孔十二面体纳米笼催化剂可降低锌-空气电池中的氧气含量
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-09-05 DOI: 10.1039/D4YA00295D
Yanan Pan, Qi Yang, Xiaoying Liu, Fan Qiu, Junjie Chen, Mengdie Yang, Yang Fan, Haiou Song and Shupeng Zhang

The coupling of multiple low-cost metals and porous nanocarbon materials aimed at replacing precious metals to enhance electrocatalytic oxygen reduction is a critical challenge in some crucial research areas. In the present study, a hollow dodecahedron nanocage catalyst (Fe3O4/CuNCs/ZnNx-PHNC) was constructed by supporting copper nanoclusters, Fe3O4 nanoparticles, and Zn–Nx after sintering and annealing through the coordination of ZIF-8 and by doping copper and iron ions. We observed that the synergy of the multi-metals in the magnetically separable heterojunction catalyst induced electron transfer and inhibited hydrogen peroxide formation, thus improving its catalytic performance for the oxygen-reduction reaction. The catalyst demonstrated a half-wave potential as high as 0.832 V and a Tafel slope of 54 mV decade−1, superior to many non-precious metal catalysts reported in the literature. The assembled Zn–air battery (ZAB) exhibited a maximum power density of 162 mW cm−2 and ultrahigh stability of >500 h at 5 mA cm−2 current density. The ZAB's excellent performance indicates its high development and practical application prospects.

低成本、多金属和多孔纳米碳材料的耦合,旨在替代贵金属增强电催化氧还原,是一些关键研究面临的重要挑战。本文利用 ZIF-8 的配位和铜、铁离子的掺杂,通过烧结退火后支撑铜纳米团簇、Fe3O4 纳米粒子和 Zn-NX 构建了十二面体空心纳米笼催化剂(Fe3O4/CuNCs/ZnNx-PHNC)。我们观察到,磁性可分离异质结催化剂中多金属的协同作用诱导了电子转移,抑制了过氧化氢的形成,从而提高了其对氧还原反应的催化性能。其半波电位高达 0.832 V,塔菲尔斜率为 54 mV/decade,优于文献中的许多非贵金属催化剂。组装后的锌空气电池(ZAB)的最大功率密度为 162 mW⸱cm-2,在 5 mA⸱cm-2电流密度条件下可保持 500 小时的超高稳定性。ZAB 的卓越性能也证明了其极高的开发和实际应用前景。
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引用次数: 0
Development of an automated SILAR method for the sustainable fabrication of BiOI/TiO2 photoanodes† 开发可持续制造生物氧化物/二氧化钛光阳极的自动化 SILAR 方法
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-09-05 DOI: 10.1039/D4YA00405A
Roberto Altieri, Fabian Schmitz, Manuel Schenker, Felix Boll, Luca Rebecchi, Pascal Schweitzer, Matteo Crisci, Ilka Kriegel, Bernd Smarsly, Derck Schlettwein, Francesco Lamberti, Teresa Gatti and Mengjiao Wang

BiOI is a promising material for use in photoelectrocatalytic water oxidation, renowned for its chemical inertness and safety in aqueous media. For device integration, BiOI must be fabricated into films. Considering future industrial applications, automated production is essential. However, current BiOI film production methods lack automation and efficiency. To address this, a continuous automated process is introduced in this study, named AutoDrop, for producing BiOI films. Autodrop results to be a fast and facile method for producing BiOI photoelectrodes. Nanostructured thin films of this layered material are prepared using a syringe pump to dispense the precursor solution onto a continuously spinning substrate. These films are integrated into a multilayered photoelectrode, featuring mesoporous TiO2 as an electron-transporting layer on top of FTO glass. In testing the photoelectrochemical performance of the BiOI/TiO2 photoelectrodes, the highest photocurrent (44 μA cm−2) is found for a heterojunction with a BiOI thickness of 320 nm. Additionally, a further protective TiO2 ultrathin layer in contact with BiOI, grown by atomic layer deposition, enhances the durability and efficiency of the photoanode, resulting in a more than two-fold improvement in photocurrent after 2 hours of continuous operation. This study advances the automation in the sustainable production of photoelectrode films and provides inspiration for further developments in the field.

BiOI 因其在水介质中的化学惰性和安全性而闻名,是一种有望用于光电催化水氧化的材料。为实现设备集成,必须将 BiOI 制成薄膜。考虑到未来的工业应用,自动化生产至关重要。然而,目前的 BiOI 薄膜生产方法缺乏自动化和效率。为解决这一问题,本研究引入了一种名为 AutoDrop 的连续自动流程,用于生产 BiOI 薄膜。结果表明,Autodrop 是一种快速、简便的生产 BiOI 光电电极的方法。使用注射泵将前驱体溶液分配到连续旋转的基底上,制备出这种层状材料的纳米结构薄膜。这些薄膜被集成到多层光电极中,其中介孔二氧化钛是 FTO 玻璃上的电子传输层。在测试 BiOI/TiO2 光电极的光电化学性能时,发现 BiOI 厚度为 320 纳米的异质结的光电流最高(44 μA cm-2)。此外,通过原子层沉积法在与 BiOI 接触处进一步生长的 TiO2 超薄保护层提高了光阳极的耐用性和效率,使其在连续工作 2 小时后的光电流提高了两倍多。这项研究推动了光电极薄膜可持续生产的自动化进程,并为该领域的进一步发展提供了灵感。
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引用次数: 0
Recent advances in in situ/operando characterization of lithium–sulfur batteries 锂硫电池原位/操作表征的最新进展
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-09-04 DOI: 10.1039/D4YA00416G
Thomas J. Leckie, Stuart D. Robertson and Edward Brightman

The lithium–sulfur battery (LSB) is a next generation energy storage technology with potential to replace lithium-ion batteries, due to their larger specific capacity, cheaper and safer manufacturing materials, and superior energy density. LSBs are a rapidly progressing topic globally, with around 1800 publications each year and the market is expected to exceed 1.7 billion USD by 2028, as such many novel strategies are being explored to develop and commercialise devices. However, significant technical challenges must be solved to engineer LSBs with commercially viable cycle life, which requires a deeper understanding of the chemical mechanisms occurring within the battery structure. In recent years in situ/operando testing of LSBs has become a popular approach for deciphering the kinetics and mechanisms of their discharge process, which is notoriously complex, and visualising the effects of mass deposition onto the electrodes and how these factors affect the cell's performance. In this review, in situ and operando studies are discussed in the context of LSBs with particular focus on spectroscopic and morphological techniques in line with trends in the literature. Additionally, some techniques have been covered which have yet to be used widely in the literature but could prove to be invaluable tools for analysis in the future. These in situ/operando techniques are becoming more widely available, and a review is useful both for the research community and industry to help accelerate the commercialisation of this next-generation technology.

锂硫电池(LSB)是下一代储能技术,具有取代锂离子电池的潜力,因为其比容量更大,制造材料更便宜、更安全,能量密度更高。LSB 在全球范围内发展迅速,每年约有 1800 篇论文发表,预计到 2028 年市场规模将超过 17 亿美元。然而,要设计出具有商业可行性循环寿命的 LSB,必须解决重大的技术难题,这就需要深入了解电池结构内发生的化学机制。近年来,LSB 的原位/操作测试已成为一种流行的方法,可用于解密其放电过程的动力学和机制(这是出了名的复杂),并直观了解质量沉积到电极上的影响以及这些因素如何影响电池的性能。本综述讨论了 LSB 的原位和操作研究,特别侧重于光谱和形态学技术,以符合文献的发展趋势。此外,本综述还介绍了一些尚未在文献中广泛使用的技术,这些技术在未来可能会成为宝贵的分析工具。这些原位/操作性技术的应用范围越来越广,对研究界和工业界进行综述非常有用,有助于加快这种下一代技术的商业化进程。
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引用次数: 0
Controlled synthesis of copper sulfide-based catalysts for electrochemical reduction of CO2 to formic acid and beyond: a review 用于将二氧化碳电化学还原为甲酸及其他物质的硫化铜相关催化剂的可控合成:综述
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-09-03 DOI: 10.1039/D4YA00302K
Anirban Mukherjee, Maryam Abdinejad, Susanta Sinha Mahapatra and Bidhan Chandra Ruidas

Converting carbon dioxide (CO2) into value-added chemicals is considered as a promising strategy to mitigate climate change. Among the various CO2 reduction techniques, electrochemical CO2 reduction (ECO2R) using renewable energy sources holds significant potential. Consequently, the design and development of electrocatalysts capable of offering both high performance and cost-effectiveness hold the potential to expedite reaction kinetics and facilitate widespread industrial adoption. In recent years, abundant copper sulfide (Cu/S)-based nanomaterials among various metal–chalcogenides have attracted extensive research interest due to their semiconductivity and low toxicity, enabling them to be used in a wide range of applications in the ECO2R field. This review highlights the progress in engineered Cu/S-based nanomaterials for ECO2R reactions and elaborates on the correlations between engineering strategies, catalytic activity, and reaction pathways. This paper also summarises the controllable synthesis methods for fabricating various state-of-the-art Cu/S-based structures and outlines their possible implementation as electrocatalysts for CO2 reduction. Finally, challenges and prospects are presented for the future development and practical applications of Cu/S-based catalysts for ECO2R to value-added chemicals.

将二氧化碳(CO2)转化为高附加值的化学品被认为是减缓气候变化的一项有前途的战略。在各种二氧化碳还原技术中,利用可再生能源进行电化学二氧化碳还原(ERCO2)具有巨大潜力。因此,设计和开发既能提供高性能又具有成本效益的电催化剂,有可能加快反应动力学,促进工业广泛采用。近年来,在各种金属钙化物中,与硫化铜(Cu/S)相关的丰富纳米材料因其半导体和低毒特性而受到广泛的研究关注,使其能够广泛应用于ERCO2领域。本综述重点介绍了用于ERCO2 反应的工程化 Cu/S 相关纳米材料的研究进展,并详细阐述了工程化策略、催化活性和反应途径之间的相互关系。论文还总结了制造各种最先进的 Cu/S 相助结构的可控合成方法,并概述了将其作为电催化剂用于二氧化碳还原的可能性。最后,还介绍了用于 ECO2R 的 Cu/S 相助催化剂在未来发展和实际应用方面的挑战和前景,以及如何将其转化为高附加值化学品。
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引用次数: 0
Electricity generation using a microbial 3D bio-anode embedded bio-photovoltaic cell in a microfluidic chamber† 利用微流控室中的微生物三维生物阳极嵌入式生物光伏电池发电
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-09-03 DOI: 10.1039/D4YA00278D
Zülal Muganlı, İsmail Bütün, Ghazaleh Gharib and Ali Koşar

New-generation sustainable energy systems serve as major tools to mitigate the greenhouse gas emissions and effects of climate change. Biophotovoltaics (BPVs) presents an eco-friendly approach by employing solar energy to ensure self-sustainable bioelectricity. In contrast to other microbial fuel cells (MFCs), carbon feedstock is not essential for generating electricity with BPVs. However, the low power outputs (μW cm−2) obtained from the current systems limit their practical applications. In this study, a new generation polydimethylsiloxane (PDMS) based BPV cell unit was developed with a 3D hydrogel scaffold-based bio-anode to enable microbial biofilm formation for substantial electron capture and extracellular electron transfer. Moreover, the fabricated device was supported using an air-cathode electrode to elevate the gas exchange, thereby enabling optimum photosynthesis. Synechocystis sp. PCC 6803 seeded the 3D bio-anode embedded BPV cell, whose electrical characteristics were analyzed under the illumination of white light as day/night cycles with continuous feeding by the microchannel. For the first five days, the results indicated that the maximum power densities were 0.0534 W m−2 for dark hours and 0.03911 W m−2 for light hours without causing any effect on the cellular morphology of the cyanobacteria. As a result, the developed hydrogel scaffold-based bio-anode embedded BPV cell led to higher power densities via enabling a simple, self-sustainable, biocompatible, and eco-friendly energy harvesting platform with a possible capability in the applications of power lab-on-a-chip (LOC), point-of-care (POC), and small-scale portable electronic devices.

新一代可持续能源系统是减缓温室气体排放和气候变化影响的主要工具。生物光电(BPV)是一种生态友好型方法,它利用太阳能确保生物电力的自我可持续性。与其他微生物燃料电池(MFCs)相比,生物光伏发电不需要碳原料。然而,现有系统的低功率输出(μW cm-2)限制了其实际应用。本研究开发了一种基于聚二甲基硅氧烷(PDMS)的新一代 BPV 单元,该单元采用三维水凝胶支架生物阳极,可形成微生物生物膜,从而实现大量电子捕获和细胞外电子传递。此外,还利用空气阴极电极支持所制造的装置,以提高气体交换,从而实现最佳光合作用。将 Synechocystis sp. PCC 6803 作为三维生物阳极嵌入式 BPV 细胞的种子,在白光的昼夜循环照射下,通过微通道持续进水,对其电学特性进行了分析。结果表明,在最初的五天中,暗时的最大功率密度为 0.0534 W m-2,亮时的最大功率密度为 0.03911 W m-2,但并未对蓝藻的细胞形态造成任何影响。因此,所开发的基于水凝胶支架的生物阳极嵌入式 BPV 电池可实现更高的功率密度,是一种简单、可自我维持、生物兼容和生态友好的能量收集平台,可应用于功率实验室芯片(LOC)、护理点(POC)和小型便携式电子设备。
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引用次数: 0
Construction of organic–inorganic hybrid composites derived from C3N5 incorporated with CeO2 for enhanced photocatalytic hydrogen evolution† 构建由 C3N5 与 CeO2 结合而成的有机无机杂化复合材料,用于增强光催化氢气进化
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-09-03 DOI: 10.1039/D4YA00476K
Ashil Augustin, Manova Santhosh Yesupatham, M. D. Dhileepan, Sanguk Son, Ezhakudiyan Ravindran, Bernaurdshaw Neppolian, Hyoung-il Kim and Karthikeyan Sekar

Energy scarcity and environmental issues can be effectively addressed via photocatalytic hydrogen production. The effective combination of semiconductor materials can prevent exciton recombination, making it a highly effective method for enhancing photocatalytic activity. This study details the synthesis of a conjugated polymer encapsulated with a metal oxide photocatalyst using a simple ex situ method. The encapsulation of the polymer with CeO2 nanoparticles resulted in exceptional performance in H2 production, exhibiting improved visible light absorption and a significant increase in charge transfer efficiency. This is attributed to the high charge transfer and reduced recombination in the composite. Moreover, photogenerated holes led to a substantial decline in the recombination rate of excitons and concomitant enhancement in the rate of photocatalytic H2 production. Markedly, the observed hydrogen evolution for 10 wt% of CeO2 doped C3N5 composites is 1256 μmol g−1 h−1, whereas for C3N5, it is 125 μmol g−1 h−1. Electrochemical analysis showed that the optimized composites exhibit a low electron–hole recombination rate, and UV-vis spectroscopic analysis showed improved visible light absorption resulting in excellent photocatalytic activity. Notably, the proposed system offers a novel strategy for hydrogen evolution via photocatalysis using CeO2/C3N5 composites. Consequently, this research offers a new perspective on the design of organo–inorganic heterostructures and introduces a novel pathway to explore their catalytic capabilities.

光催化制氢可有效解决能源短缺和环境问题。半导体材料之间的有效结合能够防止激子重组,是一种非常有效的增强光催化活性的方法。本报告采用简单的原位合成方法合成了包裹金属氧化物光催化剂的共轭聚合物。将聚合物与 CeO2 纳米粒子封装在一起后,样品对可见光的吸收得到改善,电荷转移效率显著提高,因此在生产 H2 方面表现优异。这归功于复合材料中的高电荷转移和减少的重组。光生空穴的高效转移导致激子的重组率大幅下降,光催化产生 H2 的速率大幅提高。结果表明,10 wt.% CeO2/C3N5 复合材料的氢气进化量为 1256 μmol/g/h,而 C3N5 为 125 μmol/g/h。电化学分析表明,优化后的复合材料具有较低的电子空穴重组率和更高的可见光吸收率,从而表现出优异的光催化活性。值得注意的是,该研究首次报道了利用 CeO2/C3N5 复合材料通过光催化实现氢气进化。因此,这项研究为有机无机异质结构的设计提供了一个新的视角,并将为其催化功能提供一条新的途径。
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引用次数: 0
Novel carbon-free innovation in centralised ammonia cracking for a sustainable hydrogen economy: the hybrid air-volt ammonia cracker (HAVAC) process 用于可持续氢经济的集中式氨裂解无碳创新技术:混合气体-电压氨裂解工艺(HAVAC)
IF 3.2 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-09-03 DOI: 10.1039/D4YA00483C
Chidozie Eluwah and Paul S. Fennell

The hybrid air-volt ammonia cracker (HAVAC) represents a novel approach to centralised ammonia cracking for hydrogen production, enhancing both efficiency and scalability. This novel process integrates renewable electricity and autothermal operation to crack blue or green ammonia, achieving a high thermal efficiency of 94% to 95%. HAVAC demonstrates impressive ammonia conversion rates up to 99.4% and hydrogen yields between 84% and 99.5%, with hydrogen purity of 99.99% meeting ISO 14687:2019 standards. Key innovations include the process's flexibility to operate in three modes: 100% renewable electricity, 100% air autothermal, or a hybrid approach. This versatility optimizes energy use and adapts to varying conditions. The gas heated cracker (GHC) within HAVAC efficiently reduces energy demands by utilizing waste heat. Modelled using the Aspen Plus Simulator and validated against experimental data, HAVAC's economic analysis indicates a levelized cost of hydrogen (LCOH) between $3.80 per kg-H2 and $6.00 per kg-H2. The process's environmental benefits include reduced greenhouse gas emissions and effective NOx waste management. Future research will focus on scaling up, reducing ammonia feed cost, optimizing catalysts, and enhancing waste management. HAVAC offers substantial promise for advancing hydrogen production and supporting a sustainable, carbon-free hydrogen economy. The technical and economic data generated by this analysis will assist decision-makers and researchers in advancing the pursuit of a carbon-free hydrogen economy.

混合气体-电压氨裂解器(HAVAC)是一种集中式氨裂解制氢的新方法,可提高效率和可扩展性。这种新工艺将可再生电力和自热操作整合在一起,用于裂解蓝氨或绿氨,热效率高达 94% 至 95%。HAVAC 的氨转化率高达 99.4%,氢气产量介于 84% 和 99.5% 之间,氢气纯度为 99.99%,符合 ISO 14687:2019 标准。主要创新包括该工艺可在三种模式下灵活运行:100% 可再生能源电力、100% 空气自热或混合方法。这种多功能性可优化能源利用并适应各种条件。HAVAC 中的气体加热裂解器 (GHC) 通过利用余热有效降低了能源需求。通过使用 Aspen Plus 模拟器建模并根据实验数据进行验证,HAVAC 的经济分析表明,氢气的平准化成本(LCOH)介于每千克-H2 3.80 美元和每千克-H2 6.00 美元之间。该工艺的环境效益包括减少温室气体排放和有效的氮氧化物废物管理。未来的研究重点是扩大规模、降低氨进料成本、优化催化剂和加强废物管理。HAVAC 为推进氢气生产和支持可持续的无碳氢经济带来了巨大希望。本分析所产生的技术和经济数据将有助于决策者和研究人员推动无碳氢经济的发展。
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Energy advances
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