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Unlocking the value of food waste: sustainable production of ethylene glycol over low-cost Ni–W catalysts supported on glucose-derived carbons† 释放食物垃圾的价值:利用葡萄糖衍生碳支撑的低成本 Ni-W 催化剂可持续生产乙二醇
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-09-02 DOI: 10.1039/D4SE00823E
Lucília Sousa Ribeiro, Rafael Gomes Morais, José Joaquim de Melo Órfão and Manuel Fernando Ribeiro Pereira

Food waste is abundant and holds great potential to be converted into valuable chemicals like ethylene glycol (EG), which is a key compound for the production of commodity polymers and other specialty products. Therefore, the direct conversion of food waste could represent a pivotal alternative for the sustainable production of EG. Nickel-tungsten catalysts supported on glucose-derived carbons were synthesized and evaluated for EG direct production from cellulose and cellulosic urban wastes. A remarkable yield of EG of 62% was attained directly from cellulose after 5 h, while the optimized catalyst allowed to reach notable EG yields around 40% from cellulosic wastes. Furthermore, as far as we are concerned, no previous works have reported the conversion of food wastes, such as fruit peels, directly into EG. Therefore, we report the environmentally friendly production of EG from banana peel, orange peel and spent coffee grounds with promising yields of up to 21%.

厨余垃圾数量丰富,具有将其转化为乙二醇(EG)等有价值化学品的巨大潜力,而乙二醇是生产商品聚合物和其他特种产品的关键化合物。因此,直接转化食物垃圾可能是可持续生产乙二醇的关键替代方法。我们合成并评估了以葡萄糖衍生碳为载体的镍钨催化剂,用于从纤维素和纤维素城市废物中直接生产 EG。5 小时后,直接从纤维素中获得了 62% 的显著 EG 产量,而优化后的催化剂可从纤维素废料中获得约 40% 的显著 EG 产量。此外,就我们所知,之前还没有任何关于将果皮等食物垃圾直接转化为 EG 的报道。因此,我们报告了利用香蕉皮、橘子皮和用过的咖啡渣生产 EG 的环境友好型方法,产量有望达到 21%。
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引用次数: 0
Evolving bifacial molecule strategy for surface passivation of lead halide perovskite solar cells† 用于卤化铅过氧化物太阳能电池表面钝化的不断发展的双面分子策略
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-09-02 DOI: 10.1039/D4SE01096E
Nanaki Minoi, Fumitaka Ishiwari, Takuya Omine, Kazuharu Murotani, Ryosuke Nishikubo and Akinori Saeki

A variety of passivation molecules have enhanced the performance and stability of organic–inorganic lead halide perovskite solar cells (PSCs); however, the tailoring of the design of these molecules remains largely unexplored. In this work, we propose two new classes of passivation molecules: a C2-symmetric syn-type bifacial donor–π–donor molecule and a C3-symmetric syn-type bifacial truxene. The former (PM-syn) bears hydrophobic alkylphenols and hydrophilic diethylene glycol-substituted phenyls on each face of the indenofluorene π-core. Owing to the efficient hole transfer and surface passivation by the flanked donor units, PM-syn (a racemate of enantiomers) exhibited an improved power conversion efficiency (PCE) of 18.79% and long-term stability compared with the control device (17.98%). The latter, bifacial truxene (TRX-syn), appended with three carboxyl units on one face, exhibited an improved PCE (19.76%) and stability, demonstrating the general effectiveness of the bifacial molecular concept in the passivation of PSC. Comparative spectroscopic and time-resolved studies of bifacial molecules and their anti-type analogues support our claims and provide a rich area for the design of new molecules for the modification of perovskite layers.

各种钝化分子提高了有机-无机卤化铅包晶太阳能电池(PSCs)的性能和稳定性;然而,这些分子的定制设计在很大程度上仍未得到探索。在这项工作中,我们提出了两类新的钝化分子:一种是 C2 对称合成型双向供体-π-供体分子,另一种是 C3 对称合成型双向楚克森分子。前者(PM-syn)在茚芴π核的每个面上都有疏水的烷基酚和亲水的二甘醇取代苯基。由于侧面供体单元的高效空穴传输和表面钝化作用,PM-syn(对映体的外消旋体)与对照器件(17.98%)相比,功率转换效率(PCE)提高了 18.79%,并且具有长期稳定性。后一种双面楚克森(TRX-syn)在一个面上添加了三个羧基单元,其 PCE(19.76%)和稳定性均有所提高,这表明双面分子概念在钝化 PSC 方面具有普遍的有效性。对双面分子及其反类型类似物进行的光谱和时间分辨比较研究支持了我们的观点,并为设计新的分子来修饰包晶石层提供了一个丰富的领域。
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引用次数: 0
Bioinspired photo-driven hydrogen evolution systems based on hydrogenases and their mimics 基于氢酶及其模拟物的生物启发光驱动氢进化系统
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-08-30 DOI: 10.1039/D4SE00423J
Rahat Gupta and Amlan K. Pal

The ever-growing problem of the energy crisis can be addressed with the development of sustainable and renewable sources of energy. The naturally occurring hydrogenases with their active sites provide us with a blueprint to mimic the reaction pathway and mechanism of hydrogen production. This work presents an in-depth summary of the photocatalytic hydrogen production employing 4d/5d-T-metal complexes, quantum dots, and organic dyes as photosensitizers (PSs) and hydrogenase mimics as catalysts. This review is focused on the careful design of both the PSs and catalysts to enhance the overall catalytic activity of artificial photosynthetic systems. The paths followed during the photoinduced electron transfer including the active sites of the catalysts, are discussed to guide the design of robust and efficient photocatalytic hydrogen production systems. The reduction potentials of the catalysts and PSs, change in the free energy values and density functional theory (DFT) calculations are discussed to assess the thermodynamic feasibility of the photoinduced electron transfer processes.

通过开发可持续的可再生能源,可以解决日益严重的能源危机问题。自然界存在的氢化酶及其活性位点为我们提供了模仿制氢反应途径和机制的蓝图。本研究深入总结了利用 4d/5d-T 金属复合物、量子点和有机染料作为光敏剂(PSs)以及氢酶模拟物作为催化剂的光催化制氢方法。本综述的重点是精心设计光敏剂和催化剂,以提高人工光合作用系统的整体催化活性。文章讨论了光诱导电子转移过程中的路径,包括催化剂的活性位点,以指导设计稳健高效的光催化制氢系统。讨论了催化剂和 PS 的还原电位、自由能值的变化以及密度泛函理论 (DFT) 计算,以评估光诱导电子转移过程的热力学可行性。
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引用次数: 0
Moisture-induced ionovoltaic electricity generation using lead free 2-dimensional Cs3SbBiBr9 perovskite† 利用无铅二维 Cs3SbBiBr9 包晶进行湿气诱导离子光伏发电
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-08-29 DOI: 10.1039/D4SE00997E
Ashna K. Pramod and Sudip K. Batabyal

In the field of solar energy applications, ion migration is a significant challenge. A promising solution to tackle this issue is through the Ionovoltaic Electricity Generator (IEG) effect observed in two-dimensional (2D) lead-free halide perovskite structures equipped with lateral electrodes. These devices with millimeter-spaced lateral electrodes generate electricity through moisture absorption. As moisture is absorbed, it creates an uneven distribution of ions, establishing a gradient that prompts ion migration. This migration generates a voltage difference across the electrodes, which in turn propels electrons through an external circuit, producing electrical power. Furthermore, humidity plays a crucial role in enhancing power generation by aiding in ion formation. In this study, we successfully synthesized mixed alloys of antimony and bismuth in the form of nanosheets of Cs3SbBiBr9 using a solution-based approach. The Cs3SbBiBr9 device, covering an area of 0.3 cm2 (1.5 cm × 0.2 cm), demonstrated an open-circuit voltage (Voc) of 0.22 V and a short-circuit current (Isc) of 35 μA at 85% relative humidity (RH).

在太阳能应用领域,离子迁移是一项重大挑战。要解决这一问题,一个很有前景的办法是通过在配备横向电极的二维(2D)无铅卤化物过氧化物结构中观察到的离子光伏发电(IEG)效应。这些横向电极间距为毫米的装置通过吸湿发电。当水分被吸收时,会造成离子分布不均,形成一个梯度,促使离子迁移。这种迁移会在电极上产生电压差,进而推动电子通过外部电路,产生电能。此外,湿度通过帮助离子形成,在提高发电量方面起着至关重要的作用。在本研究中,我们采用溶液法成功合成了 Cs3SbBiBr9 纳米片状的锑铋混合合金。Cs3SbBiBr9 器件面积为 0.3 cm2(1.5 cm × 0.2 cm),在相对湿度为 85% 的条件下,开路电压 (Voc) 为 0.22 V,短路电流 (Isc) 为 35 μA。
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引用次数: 0
Critical insights into eutectic molten hydroxide electrolysis for sustainable green hydrogen production 共晶熔融氢氧化物电解用于可持续绿色制氢的关键见解
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-08-29 DOI: 10.1039/D4SE01060D
Farooq Sher, Imane Ziani, Nawar K. Al-Shara, Alexander Chupin, Nađa Horo, Bohong Wang, Saba Rahman, Bilal Fareed and Monica R. Nemţanu

In addressing global energy demands, the focus on hydrogen gas production from renewable sources intensifies. This research review investigates hydrogen production via steam splitting using eutectic molten hydroxide (NaOH–KOH%) electrolysis, a promising solution for escalating energy needs. A pivotal aspect involves developing a novel reference electrode for eutectic molten hydroxide, enveloping Ni/Ni(OH)2 with an alumina or mullite tube ionic membrane. The mullite-covered electrode proves stable and reusable from 225 to 300 °C, showcasing a novel advancement in electrochemical stability. Compared to silver and platinum quasi-reference electrodes, the designed reference electrode demonstrates superior stability and efficacy in controlling the platinum working electrode, marking a significant innovation. Moreover, an intriguing cyclic voltammetry study examines different working electrodes, including Ni, Pt, Ag, Mo, and stainless steel (SS) in eutectic molten hydroxide at different temperature conditions. The observed reduction potential for hydrogen evolution follows the order: Ni > Pt > Ag > SS > Mo, corroborated by chronoamperometry, underscoring the reliability of the findings. In the pursuit of high-temperature eutectic molten hydroxide electrolysis to split steam into hydrogen fuel, cathodes of nickel, platinum, and stainless steel are deployed alongside stainless steel and graphite anodes. Operating within the temperature range of 225 to 300 °C and applying voltages ranging from 1.5 to 2.5 V, stainless steel as an anode yields impressive current efficiencies at 300 °C: 90.5, 80 and 68.6% for nickel, stainless steel, and platinum cathodes, respectively. This study positions steam splitting via molten hydroxides as a promising alternative for hydrogen production, poised for integration with renewable energy sources, marking a transformative step in sustainable energy practices.

为满足全球能源需求,利用可再生能源生产氢气日益受到关注。本研究综述探讨了利用共晶熔融氢氧化物(NaOH-KOH%)电解法通过蒸汽裂解制取氢气的方法,这是一种有望满足日益增长的能源需求的解决方案。其中一个关键方面是为共晶熔融氢氧化物开发一种新型参比电极,用氧化铝或莫来石管离子膜包裹 Ni/Ni(OH)2。事实证明,莫来石包裹的电极在 225 至 300 °C 的温度范围内稳定且可重复使用,在电化学稳定性方面取得了新的进展。与银和铂准参比电极相比,所设计的参比电极在控制铂工作电极方面表现出卓越的稳定性和功效,是一项重大创新。此外,一项引人入胜的循环伏安法研究在不同温度条件下对共晶熔融氢氧化物中的不同工作电极进行了检测,包括镍、铂、银、钼和不锈钢(SS)。观察到的氢演化还原电位遵循以下顺序:在进行高温共晶熔融氢氧化物电解将蒸汽转化为氢燃料的过程中,镍、铂和不锈钢阴极与不锈钢和石墨阳极一起使用。不锈钢阳极的工作温度范围为 225 至 300 °C,电压范围为 1.5 至 2.5 V,在 300 °C时的电流效率令人印象深刻:镍、不锈钢和铂阴极的电流效率分别为 90.5%、80% 和 68.6%。这项研究将通过熔融氢氧化物进行蒸汽裂解定位为一种前景广阔的制氢替代方法,有望与可再生能源相结合,标志着可持续能源实践迈出了变革性的一步。
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引用次数: 0
Near-infrared driven photocatalytic hydrogen production from ammonia borane hydrolysis using heterostructure-upconverted nanoparticles† 利用异质结构上转换纳米粒子在氨硼烷水解过程中进行近红外光催化制氢
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-08-28 DOI: 10.1039/D4SE01047G
Bushra Maryam, Muhammad Asim, Hamna Qayyum, Lun Pan, Ji-Jun Zou and Xianhua Liu

This study presents a novel approach to hydrogen evolution through ammonia borane dehydrogenation, utilizing the unique properties of upconverted nanoparticles (UCNPs) and safe, abundant near-infrared (NIR) light. By converting low-energy 980 nm NIR photons into high-energy visible photons, UCNPs offer a significant enhancement in catalytic activity. The fabrication of polystyrene-incorporated UCNPs (PS@UCNPs) prevents catalyst agglomeration and breakage, resulting in a 35-fold increase in activity compared to bare UCNPs. This increase is due to the high-energy emitted photons providing sufficient energy for hydrogen evolution, thereby reducing catalyst costs and eliminating the need for intermediate catalysts. The study also explores platinum-coated UCNPs (Pt@UCNPs), which increase photon absorption by platinum nanoparticles, significantly boosting photocatalytic performance. Pt@UCNPs demonstrated 25 times higher activity than PS@UCNPs, attributed to the unique properties of Pt nanoparticles. The activation energies for PS@UCNPs and Pt@UCNPs were 27.5 kJ mol−1 and 48.8 kJ mol−1, respectively, highlighting the synergistic effect of UCNPs utilizing NIR light and Pt utilizing visible light. Reaction kinetics indicated that hydrogen evolution rates increased with both catalyst and ammonia borane concentrations under NIR light. Recyclability tests confirmed the superior stability and durability of PS@UCNPs over Pt@UCNPs, with consistent hydrogen evolution rates across five cycles and minimal degradation. These findings position PS@UCNPs as a robust catalyst system with significant potential for long-term applications, contributing to the broader field of photochemical catalysis and inspiring further innovations in renewable energy systems. As materials and technologies continue to evolve, NIR-activated photocatalytic processes are expected to play a crucial role in the transition to a sustainable energy future, significantly impacting renewable energy and green chemistry.

本研究利用上转换纳米粒子(UCNPs)的独特性质和安全、丰富的近红外(NIR)光,提出了一种通过氨硼烷脱氢实现氢进化的新方法。通过将低能量的 980 纳米近红外光子转化为高能量的可见光光子,UCNPs 可显著提高催化活性。聚苯乙烯掺杂 UCNPs(PS@UCNPs)的制造可防止催化剂团聚和断裂,从而使催化活性比裸 UCNPs 提高了 35 倍。这种提高是由于高能发射的光子为氢气进化提供了足够的能量,从而降低了催化剂成本,并消除了对中间催化剂的需求。该研究还探讨了铂涂层 UCNPs(Pt@UCNPs),它能增加铂纳米粒子对光子的吸收,从而显著提高光催化性能。Pt@UCNPs 的活性比 PS@UCNPs 高 25 倍,这归功于铂纳米粒子的独特性质。PS@UCNPs 和 Pt@UCNPs 的活化能分别为 27.5 kJ mol-1 和 48.8 kJ mol-1,凸显了利用近红外光的 UCNPs 和利用可见光的 Pt 的协同效应。反应动力学表明,在近红外光下,氢气进化速率随催化剂和硼烷氨浓度的增加而增加。可回收性测试证实,与 Pt@UCNPs 相比,PS@UCNPs 具有更高的稳定性和耐久性,在五个循环中氢进化率保持一致,降解程度极低。这些发现将 PS@UCNPs 定义为具有长期应用潜力的稳健催化剂体系,有助于拓展光化学催化领域,并激发可再生能源系统的进一步创新。随着材料和技术的不断发展,近红外激活的光催化过程有望在向可持续能源未来过渡的过程中发挥关键作用,对可再生能源和绿色化学产生重大影响。
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引用次数: 0
A new type of pyranthrene-based copolymer as a promising hole-transport material for perovskite solar cells† 一种新型吡喃蒽基共聚物是一种很有前景的过氧化物太阳能电池空穴传输材料
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-08-28 DOI: 10.1039/D4SE00481G
Azat F. Akbulatov, Ekaterina A. Khakina, Nikita A. Emelianov, Olga A. Kraevaya, Lyubov A. Frolova and Pavel A. Troshin

Perovskite solar cells (PSCs) with an n–i–p configuration have demonstrated rapid progress in the past few years, though the most efficient devices were made using a doped small molecular hole-transport material, spiro-OMeTAD, which deteriorates their long-term stability. To address this problem, dopant-free hole transport materials should be developed. Herein, we present the synthesis and characterization of poly(4-(5′-(16-(3,4′-bis(2-ethylhexyl)-[2,2′-bithiophen]-5-yl)pyranthrene-8-yl)-3′,4-bis(2-ethylhexyl)-[2,2′-bithiophen]-5-yl)benzo[c][1,2,5]thiadiazole) (PATTBTT), which is considered as a promising hole-transport material for PSCs. The designed copolymer PATTBTT delivered a power conversion efficiency of 17.6% in PSCs, which was higher than those obtained for reference devices fabricated using dopant-free polytriarylamine-based hole-transport materials. These results demonstrate that pyranthrene-based conjugated polymers represent a promising new family of materials for high-efficiency perovskite solar cells.

采用 ni-i-p 配置的过氧化物太阳能电池(PSCs)在过去几年中取得了飞速发展,尽管最高效的设备是使用掺杂小分子空穴传输材料螺-OMeTAD 制成的,但这种材料会降低设备的长期稳定性。为解决这一问题,应开发不含掺杂剂的空穴传输材料。在此,我们介绍了聚(4-(5′-(16-(3,4′-双(2-乙基己基)-[2,2′-双噻吩]-5-基)吡喃蒽-8-基)-3′、4-双(2-乙基己基)-[2,2′-双噻吩]-5-基)苯并[c][1,2,5]噻二唑)(PATTBTT)的共聚物,它被认为是一种很有前途的 PSC 孔传输材料。设计的共聚物 PATTBTT 在 PSC 中的功率转换效率为 17.6%,高于使用无掺杂剂的聚三芳基胺空穴传输材料制造的参考器件。这些结果表明,基于吡喃蒽的共轭聚合物是一种很有前途的新型高效包晶体太阳能电池材料。
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引用次数: 0
Multifunctioning graphene oxide capping layer for highly efficient and stable PEDOT:PSS–silicon hybrid solar cells† 用于高效稳定 PEDOT:PSS 硅混合太阳能电池的多功能氧化石墨烯封盖层
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-08-27 DOI: 10.1039/D4SE00889H
Ruchi K. Sharma, Avritti Srivastava, Urvashi Punia, Riya Bansal, Pukhraj Prajapat, Govind Gupta and Sanjay K. Srivastava

Hybrid heterojunction solar cells (HHSCs) of an organic conjugate polymer, namely, poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) and silicon have received extensive attention due to their high efficiency (PCE) and low-temperature processing. However, effective collection of charge carriers from the PEDOT:PSS/n-Si interface is a challenging task due to various defects and low band offset at the interface. The current study explores ways of overcoming the limitations of HHSCs and unveils the potential of solution-processed graphene oxide (GO) thin capping layer for achieving high-efficiency and stable PEDOT:PSS/n-Si HHSCs. It also unveils the GO-induced tuning of the band bending at the interface and thus improved carrier selection. Moreover, it facilitated improved charge transportation in the PEDOT:PSS via screening the PEDOT–PSS interaction, as evidenced by a significant improvement (>2-fold) in the electrical conductivity of the PEDOT:PSS layer after applying the GO layer. The integration of the GO capping layer reduced the optical reflection to <8% and enhanced the Si surface passivation by >2 fold. The cumulative effect of GO capping led to a ∼2.4% absolute enhancement in the PCE with respect to the device without any GO layer. The champion GO/PEDOT:PSS/n-Si HHSCs exhibited a PCE of 11.66% in a simple device design on a low-cost solar-grade Si wafer. Moreover, the GO capping facilitated environment protection to the PEDOT:PSS, increasing the stability of the device under atmospheric conditions, thus revealing the great potential of the thin GO layer for highly efficient and stable HHSCs.

有机共轭聚合物聚(3,4-乙烯二氧噻吩):聚(苯乙烯磺酸)(PEDOT:PSS)与硅的混合异质结太阳能电池(HHSCs)因其高效率(PCE)和低温加工而受到广泛关注。然而,由于 PEDOT:PSS/n-Si 界面存在各种缺陷和低带偏移,从该界面有效收集电荷载流子是一项具有挑战性的任务。目前的研究探索了克服 HHSCs 限制的方法,并揭示了溶液加工氧化石墨烯(GO)薄封层在实现高效稳定的 PEDOT:PSS/n-Si HHSCs 方面的潜力。它还揭示了由 GO 引发的界面带弯曲调整,从而改善了载流子选择。此外,通过筛选 PEDOT-PSS 相互作用,它还有助于改善 PEDOT:PSS 中的电荷传输,这体现在涂覆 GO 层后 PEDOT:PSS 层的电导率显著提高(2 倍)。加入 GO 盖层后,光学反射率降低到了 8%,硅表面钝化效果提高了 2 倍。与没有任何 GO 层的器件相比,GO 覆盖层的累积效应使 PCE 绝对值提高了 2.4%。获得冠军的 GO/PEDOT:PSS/n-Si HHSCs 在低成本太阳能级硅晶片上采用简单的器件设计,显示出 11.66% 的 PCE。此外,GO 覆层还有助于保护 PEDOT:PSS,提高器件在大气条件下的稳定性,从而揭示了薄 GO 层在高效、稳定的 HHSCs 方面的巨大潜力。
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引用次数: 0
Correction: Tribo-piezoelectric nanogenerators for energy harvesting: a first-principles study 更正:用于能量收集的三压电纳米发电机:第一原理研究
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-08-27 DOI: 10.1039/D4SE90068E
Jemal Yimer Damte and Jiri Houska

Correction for ‘Tribo-piezoelectric nanogenerators for energy harvesting: a first-principles study’ by Jemal Yimer Damte et al., Sustainable Energy Fuels, 2024, https://doi.org/10.1039/D4SE00498A.

对 Jemal Yimer Damte 等人撰写的 "用于能量收集的三压电纳米发电机:第一原理研究 "的更正,《可持续能源燃料》,2024 年,https://doi.org/10.1039/D4SE00498A。
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引用次数: 0
Cr-doped CoFe2O4 nanorod array modified by oxygen vacancy-rich cerium oxide as an efficient bifunctional total water splitting catalyst† 富氧空位氧化铈修饰的铬掺杂 CoFe2O4 纳米棒阵列作为高效双功能全水分离催化剂
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-08-27 DOI: 10.1039/D4SE00966E
Yulin Duan, Zhengang Guo, Hua-nan Zhang, Tingting Wang and Jifan Zhang

Highly efficient and stable bifunctional electrocatalysts for total water splitting are crucial for the realization of large-scale hydrogen production. In this study, we successfully synthesized CeOx-modified CoCryFe2−yO4 nanorod array structures on a nickel foam substrate via two-step hydrothermal method followed by calcination. It is demonstrated that Cr doping increases the electrical conductivity of the catalyst, which allows for a larger number of electrochemically accessible active sites at the catalyst terminals, thereby improving its activity. Modification of the CoCryFe2−yO4/NF surface with oxygen vacancy-rich CeOx resulted in a highly efficient and stable bifunctional catalyst (CoCryFe2−yO4@CeOx/NF), and the exceptional bifunctional activity and stability can be attributed to: (i) Cr doping and CeOx modification induced a self-assembly transformation of the catalyst morphology from a nanosphere structure to a nanorod array structure, resulting in an increased specific surface area; (ii) the high conductivity especially in CoCr0.6Fe1.4O4, allows electrochemical access to a greater number of active sites at the catalyst periphery; (iii) the introduction of abundant oxygen vacancies by CeOx modification, which alters the electronic structure of CoCryFe2−yO4, leading to electron redistribution of Co, Cr and Fe, shifting them to higher oxidation states favorable for catalytic reactions. This promotes the formation of highly catalytically active metal oxyhydroxides on the CoCryFe2−yO4 surface during the OER process, thereby enhancing the catalytic efficiency.

高效稳定的全水分离双功能电催化剂对于实现大规模制氢至关重要。在本研究中,我们通过两步水热法和煅烧法在泡沫镍基底上成功合成了 CeOx 改性 CoCryFe2-yO4 纳米棒阵列结构。研究表明,铬的掺杂增加了催化剂的导电性,这使得催化剂终端有更多的电化学可及活性位点,从而提高了催化剂的活性。用富含氧空位的 CeOx 对 CoCryFe2-yO4/NF 表面进行修饰,可得到高效稳定的双功能催化剂(CoCryFe2-yO4@CeOx/NF),其优异的双功能活性和稳定性可归因于(i) Cr 掺杂和 CeOx 改性诱导了催化剂形态从纳米球结构向纳米棒阵列结构的自组装转变,从而增加了比表面积;(ii) CoCr0.6Fe1.4O4 的高电导率使其能够进行电化学反应。4O4 中的高导电性,使催化剂外围有更多的活性位点可以进行电化学处理;(iii) 通过 CeOx 改性引入大量的氧空位,改变了 CoCryFe2-yO4 的电子结构,导致 Co、Cr 和 Fe 的电子重新分布,使它们转移到有利于催化反应的高氧化态。这促进了 OER 过程中 CoCryFe2-yO4 表面高催化活性金属氧氢氧化物的形成,从而提高了催化效率。
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引用次数: 0
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Sustainable Energy & Fuels
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