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Boosting the performance of aqueous zinc-ion battery by regulating the electrolyte solvation structure 通过调节电解质溶解结构提高锌离子水电池的性能
Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-02-21 DOI: 10.1002/eom2.12438
Xingxing Wu, Yufan Xia, Shuang Chen, Zhen Luo, Xuan Zhang, Muhammad Wakil Shahzad, Ben Bin Xu, Hongge Pan, Mi Yan, Yinzhu Jiang

The practical implementation of aqueous Zn-ion batteries (ZIBs) for large-scale energy storage is impeded by the challenges of water-induced parasitic reactions and uncontrolled dendrite growth. Herein, we propose a strategy to regulate both anions and cations of electrolyte solvation structures to address above challenges, by introducing an electrolyte additive of 3-hydroxy-4-(trimethylammonio)butyrate (HTMAB) into ZnSO4 electrolyte. Consequently, the deposition of Zn is significantly improved leading to a highly reversible Zn anode with paralleled texture. The Zn/Zn cells with ZnSO4/HTMAB exhibit outstanding cycling performance, showcasing a lifespan exceeding 7500 h and an exceptionally high accumulative capacity of 16.47 Ah cm−2. Zn/NaV3O8·1.5H2O full cell displays a specific capacity of ~130 mAh g−1 at 5 A g−1 maintaining a capacity retention of 93% after 2000 cycles. This work highlights the regulation on both cations and anions of electrolyte solvation structures in optimizing interfacial stability during Zn plating/stripping for high performance ZIBs.

由于水引起的寄生反应和不受控制的枝晶生长等难题,阻碍了用于大规模储能的水性锌离子电池(ZIBs)的实际应用。在此,我们提出了一种通过在 ZnSO4 电解质中引入 3-羟基-4-(三甲基氨基)丁酸盐(HTMAB)电解质添加剂来调节电解质溶解结构中阴阳离子的策略,以应对上述挑战。因此,锌的沉积得到了显著改善,从而形成了具有平行纹理的高度可逆锌阳极。采用 ZnSO4/HTMAB 的锌/锌电池表现出卓越的循环性能,寿命超过 7500 小时,累积容量高达 16.47 Ah cm-2。Zn/NaV3O8-1.5H2O 全电池在 5 A g-1 条件下显示出 ~130 mAh g-1 的比容量,在循环 2000 次后保持 93% 的容量。这项研究强调了电解质溶解结构对阳离子和阴离子的调节作用,从而在锌电镀/剥离过程中优化界面稳定性,实现高性能 ZIB。
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引用次数: 0
Efficient near-infrared emission in lanthanum ion doped double perovskite Cs2NaScCl6 via Cr3+ sensitization under visible light excitation 可见光激发下通过 Cr3+ 敏化掺杂镧离子的双包晶 Cs2NaScCl6 中的高效近红外发射
Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-01-25 DOI: 10.1002/eom2.12437
Weiguo Huang, Hui Peng, Jinling Huang, Ye Yang, Qilin Wei, Bao Ke, Muhammad Sheraz Khan, Jialong Zhao, Bingsuo Zou

Herein, we synthesized Cr3+/Ln3+ (Er3+, Tm3+)-codoped rare earth-based Cs2NaScCl6 double perovskite, and the near-infrared emission of Ln3+ can be excited by visible light through the energy transfer (ET) from Cr3+ to Ln3+. Moreover, there are two independent emission bands, which stems from 4T2 → 4A2 transition of Cr3+ (970 nm) and f-f transition of Ln3+ (1542 nm for Er3+ and 1220 nm for Tm3+), respectively. Particularly, both compounds have ultra-high photoluminescence quantum yield (PLQY) of 60% for 10%Cr3+/6%Er3+-codoped Cs2NaScCl6 (Er3+ emission: ∼26%) and 68% for 10%Cr3+/4.5%Tm3+-codoped Cs2NaScCl6 (Tm3+ emission: ∼56%), which can be attributed to the ultra-high ET efficiency from Cr3+ to Ln3+ and the similar ionic activity of Sc3+ and Ln3+ allowing more dopants enter the host lattice. Considering the excellent stability of the samples, we demonstrated Cr3+/Tm3+-codoped Cs2NaScCl6 in the applications of near-infrared imaging and night vision. Finally, we reported 10%Cr3+/4.5%Tm3+/9%Er3+-tridoped Cs2NaScCl6 and further applied it for optical thermometry.

在此,我们合成了掺杂稀土的Cs2NaScCl6双包晶石Cr3+/Ln3+(Er3+,Tm3+),通过Cr3+到Ln3+的能量转移(ET),Ln3+的近红外发射可以被可见光激发。此外,还有两条独立的发射带,分别源于 Cr3+ 的 4T2 → 4A2 转变(970 nm)和 Ln3+ 的 f-f 转变(Er3+ 为 1542 nm,Tm3+ 为 1220 nm)。特别是,这两种化合物都具有超高的光致发光量子产率(PLQY),10%Cr3+/6%Er3+掺杂的 Cs2NaScCl6 为 60%(Er3+ 发射:∼26%),10%Cr3+/4.5%Tm3+掺杂的 Cs2NaScCl6(Tm3+发射率:∼56%),这可归因于从 Cr3+ 到 Ln3+ 的超高 ET 效率,以及 Sc3+ 和 Ln3+ 相似的离子活性允许更多的掺杂剂进入宿主晶格。考虑到样品的出色稳定性,我们在近红外成像和夜视应用中展示了 Cr3+/Tm3+ 掺杂的 Cs2NaScCl6。最后,我们报告了 10%Cr3+/4.5%Tm3+/9%Er3+掺杂的 Cs2NaScCl6,并将其进一步应用于光学测温。
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引用次数: 0
Morphological modulation enabled by non-halogenated solvent-processed simple solid additives for high-efficiency organic solar cells 通过非卤化溶剂加工的简单固体添加剂实现形态调节,用于高效有机太阳能电池
Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-01-24 DOI: 10.1002/eom2.12436
Muhammad Haris, Du Hyeon Ryu, Zakir Ullah, Bong Joo Kang, Nam Joong Jeon, Seungjin Lee, Hang Ken Lee, Sang Kyu Lee, Jong-Cheol Lee, Hyung-Wook Kwon, Won Suk Shin, Chang Eun Song

The simple-structural and volatile solid additive 1,4-dibromobenzene (DBrB) can outperform organic solar cells (OSCs) fabricated with 1,4-diiodobenzene and 1,4-dichlorobenzene in terms of power conversion efficiency (PCE). A remarkable PCE of 17.0% has been achieved in a binary OSC based on DBrB-optimized photoactive materials processed from non-halogenated solvents, which is mainly attributed to the formation of a three-dimensional interpenetrating network and the orderly arrangement of the photoactive materials by improving the intermolecular interaction. This optimized morphology enables efficient charge transfer/transport as well as suppressed charge recombination, resulting in the simultaneous increase in all photovoltaic parameters. More importantly, we demonstrate that non-halogenated solvent-processed DBrB enabled PM6:Y6-HU OSCs with an impressive PCE of 18.6%, which is the highest efficiency yet reported for binary OSCs. This study suggests that the novel DBrB volatile solid additive is an effective approach to optimizing the morphology and thereby improves the photovoltaic performance of OSCs.

结构简单且易挥发的固体添加剂 1,4-二溴苯(DBrB)在功率转换效率(PCE)方面优于用 1,4-二碘苯和 1,4-二氯苯制造的有机太阳能电池(OSC)。基于 DBrB 优化光活性材料的二元 OSC 实现了 17.0% 的出色 PCE,这主要归功于通过改善分子间相互作用形成的三维互穿网络和光活性材料的有序排列。这种优化的形态实现了高效的电荷转移/传输,并抑制了电荷重组,从而同时提高了所有光伏参数。更重要的是,我们证明了非卤化溶剂处理的 DBrB 使 PM6:Y6-HU OSCs 的 PCE 达到了令人印象深刻的 18.6%,这是目前报道的二元 OSCs 的最高效率。这项研究表明,新型 DBrB 挥发性固体添加剂是优化形态的有效方法,从而提高了 OSC 的光伏性能。
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引用次数: 0
Frontier sustainable nanotechnology of South Korea today 当今韩国的前沿可持续纳米技术
Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-01-16 DOI: 10.1002/eom2.12435
Il Jeon, Youn Sang Kim, Sungjoo Lee
<p>Nanotechnology sits at the heart of propelling a sustainable society, brandishing the power to revolutionize a raft of sectors, notably energy, the environment, materials, health, and agriculture. This field is integral to the sustainability agenda, sharply reducing waste, conserving energy, and minimizing the ecological imprint of human endeavors. In these domains, South Korea demonstrates formidable strengths in nano-energy, environmental technology, and the development of sophisticated nanomaterials. Particularly in renewable energy, nanotechnology markedly bolsters the efficacy of solar cells and batteries, while in environmental pursuits, it facilitates the utilization of nanomaterials for pollution mitigation and the creation of energy-efficient semiconductors. The extensive national nanotechnology strategy encompasses sectors from nano-elementary to nano-manufacturing, nano-bio, and nano-energy/environment, underscoring South Korea's commitment to a significant stake in the international market.</p><p>The commitment of South Korea to sustainable nanotechnology is vividly reflected in its national policy. Within the framework of the Green New Deal, the country is championing a holistic initiative that envisages the creation of employment and stimulation of economic growth through eco-friendly policies and technological innovations. The Deal, with a budget of approximately £104 billion by 2025, is poised to invigorate key sectors such as green mobility and intelligent healthcare. It is underpinned by a strategy to intensify renewable energy, enhance green infrastructure, and revitalize the industrial sphere, further sweetened with incentives for electric and hydrogen fuel-cell vehicles. South Korea's substantial investment in nanotechnology research and development, demonstrated through a meticulous strategic roadmap and proactive engagement in global symposia, affirms its influential position in the nanotech sphere. For example, the NANO KOREA Symposium stands as a testament to this, with the 2023 event being a crucible of cross-disciplinary progress themed “Nanodevice: Evolving into Intelligent Semiconductors,” a clear signal that South Korea is critically influencing the course of global nanotechnology innovation.</p><p>Hence, this special issue is a showcase of the forefront of nanotechnological research emanating from South Korea, brought forth by the leading minds from the country's foremost institutions. In line with the 2022 Times Higher Education (THE) University Rankings, we have sourced contributions from Seoul National University (SNU), Korea Advanced Institute of Science and Technology (KAIST), and Sungkyunkwan University (SKKU), which stand at the vanguard of this field. Esteemed colleagues, including five professors from SNU, a pair from KAIST, and a sextet from SKKU, have lent their expertise to this publication. Enclosed within are five original research articles alongside seven critical reviews, spanning a range of subje
纳米技术是推动可持续发展社会的核心,它能给能源、环境、材料、健康和农业等众多领域带来革命性的变化。这一领域是可持续发展议程不可或缺的一部分,它能大幅减少浪费、节约能源,并最大限度地减少人类活动对生态环境造成的影响。在这些领域,韩国在纳米能源、环境技术和尖端纳米材料的开发方面展现出强大的实力。特别是在可再生能源领域,纳米技术显著提高了太阳能电池和电池的效率;在环保领域,纳米技术促进了纳米材料在减轻污染和制造高能效半导体方面的应用。广泛的国家纳米技术战略涵盖了从纳米元素到纳米制造、纳米生物和纳米能源/环境等领域,突出了韩国在国际市场上占据重要地位的承诺。在 "绿色新政 "的框架内,韩国正在倡导一项综合举措,设想通过生态友好型政策和技术创新来创造就业机会和刺激经济增长。到 2025 年,"绿色新政 "的预算将达到约 1,040 亿英镑,将为绿色交通和智能医疗等关键领域注入活力。该协议以强化可再生能源、加强绿色基础设施和振兴工业领域的战略为基础,并为电动汽车和氢燃料电池汽车提供进一步的优惠政策。韩国在纳米技术研发方面的大量投资,通过精心制定的战略路线图和积极参加全球研讨会得到了证明,这也肯定了韩国在纳米技术领域的影响力。例如,NANO KOREA(韩国纳米研讨会)就证明了这一点,2023 年的研讨会将以 "纳米设备:向智能半导体发展 "为主题,成为跨学科进步的熔炉:因此,本特刊展示了韩国最前沿的纳米技术研究成果,这些成果都是由韩国最重要机构的领军人物带来的。根据 2022 年泰晤士高等教育(THE)大学排名,我们选取了首尔国立大学(SNU)、韩国科学技术院(KAIST)和成均馆大学(SKKU)等在该领域处于领先地位的院校的文章。包括韩国国立科学大学(SNU)的五位教授、韩国科学技术院(KAIST)的一对教授和韩国成均馆大学(SKKU)的六位教授在内的多位知名同行为本出版物提供了他们的专业知识。本刊收录了五篇原创研究文章和七篇评论性综述,内容涵盖了从过氧化物太阳能电池和电池的开发到前沿纳米材料在半导体中的应用等一系列主题,所有这些都与培育可持续发展的社会息息相关。这些文章代表了材料科学领域的集体努力,强调以创新提高能源效率、可持续性和环境再生。这些文章表明,材料科学领域正在进行强有力的跨学科研究,努力拓展能源存储和发电的可能性,同时满足对更多无害生态能源解决方案的迫切需求。我们对所有投稿作者、同行评审员和 EcoMat 编辑团队表示衷心感谢,感谢他们为实现本特刊所做的宝贵贡献和坚定支持。特别要感谢香港理工大学总编辑郑子健教授和执行主编卢伟深博士的不懈协助。我们殷切希望,本期特刊不仅能向读者介绍最新进展,还能激发读者对这一极其重要领域的高度关注。
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引用次数: 0
A flexible transparent graphene/metal–organic framework complex hybrid chemical sensor for highly sensitive ethanol detection 用于高灵敏度乙醇检测的柔性透明石墨烯/金属有机框架复合杂化传感器
Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-01-02 DOI: 10.1002/eom2.12433
Yong Hee Kim, Chang Ho Choi, Hyun Woo Song, Eun Kwang Lee, Dong-Pyo Kim, Joon Hak Oh

High-performance flexible and transparent chemical sensors are key to achieving wearable electronics. Graphene with high transmittance and electrical properties is a suitable material for flexible and transparent chemical sensors. However, graphene has low detectivity to chemical substances. Here, we report hybrid chemical sensors fabricated by introducing a highly flat and smooth metal–organic framework (MOF) on graphene. The graphene chemical sensors functionalized with MOF on SiO2/Si wafer exhibit 22 times higher sensitivity of 6.07 μA ppm−1 in detecting ethanol than that of pristine graphene transistors of 0.28 μA ppm−1 and a low detection limit of 1 ppm. Furthermore, a flexible transparent 7 × 7 chemical sensor array exhibits great driving stability after the bending cycles of 105 at a bending radius of 1.0 mm and shows sensitivity of 0.11 μA ppm−1. Our findings demonstrate an efficient way to improve the chemical sensing ability of graphene for application in wearable chemical sensors.

高性能柔性透明化学传感器是实现可穿戴电子设备的关键。石墨烯具有高透光率和电气特性,是柔性透明化学传感器的合适材料。然而,石墨烯对化学物质的检测率较低。在此,我们报告了通过在石墨烯上引入高度平整光滑的金属有机框架(MOF)而制造的混合化学传感器。在二氧化硅/硅晶片上用 MOF 功能化的石墨烯化学传感器检测乙醇的灵敏度为 6.07 μA ppm-1,比原始石墨烯晶体管的 0.28 μA ppm-1 高出 22 倍,检测限低至 1 ppm。此外,柔性透明 7 × 7 化学传感器阵列在弯曲半径为 1.0 毫米、弯曲次数为 105 次后表现出极高的驱动稳定性,灵敏度为 0.11 μA ppm-1。我们的研究结果表明,提高石墨烯的化学传感能力是应用于可穿戴化学传感器的有效方法。
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引用次数: 0
Natural polymers as sustainable precursors for scalable production of N/SOx doped carbon material enabling high-performance supercapacitors 以天然聚合物为可持续前体,规模化生产掺杂 N/SOx 的碳材料,实现高性能超级电容器
Q1 CHEMISTRY, PHYSICAL Pub Date : 2023-12-29 DOI: 10.1002/eom2.12434
Syed Comail Abbas, Zifeng Hua, Qidu Deng, Md Sohel Ahommed, Jiajia Guo, Hai Huang, Xiaojuan Ma, Shilin Cao, Yonghao Ni

Natural polymers-based carbon electrodes have gained significant research attention for next-generation portable supercapacitors. Herein, present an environmentally benign and novel approach for the synthesis of N/S-Ox carbon material derived from natural polymers on gram scale. By capitalizing the synergistic effect of sulfonated lignin and amino-containing chitosan, this methodology produces a straightforward, low-budget, and scalable process. The incorporation of sulfonate motifs from lignin contributes to the formation of C-SOx moieties and multi-porous architecture with a high surface area. Simultaneously, amino groups in chitosan induce nitrogen doping, enhancing conductivity, and wettability. The resulting N/SOx carbon material exhibits a micro/meso-porous architecture, facilitating electrolyte diffusion, and demonstrating improved rate capability and pseudocapacitance via Faradaic redox reactions. The N/SOx carbon material showcases notable capacitance (392 F g−1 at 1 Ag−1) as compared with the reported carbon materials form biomass and outstanding cyclic stability (94.8% retention after 5000 cycles). By optimizing various chitosan mass ratios, the most effective N/SOx carbon material SNACM = S/N-doped activated carbon material (SNACM-2) was produced using a lignin: chitosan sample ratio of 1:2 for symmetric supercapacitors. Furthermore, the quasi-solid-state symmetric supercapacitors based on SNACM-2 exhibit an excellent specific capacitance of 142 F g−1 at 1 A g−1, coupled with outstanding flexibility. The SNACM-2 demonstrates a high-energy density of 9.8 W h kg−1 at a power density of 0.5 kW kg−1. This study presents a successful strategy for transforming low-valued, eco-friendly natural polymers into renewable, high-performance carbon materials for supercapacitors.

基于天然聚合物的碳电极在下一代便携式超级电容器的研究中备受关注。本文介绍了一种以克为单位从天然聚合物中合成 N/S-Ox 炭材料的无害环境的新方法。通过利用磺化木质素和含氨基壳聚糖的协同效应,该方法可实现直接、低成本和可扩展的工艺。木质素中的磺酸基团有助于形成 C-SOx 分子和具有高比表面积的多孔结构。同时,壳聚糖中的氨基基团诱导氮掺杂,增强了导电性和润湿性。由此产生的 N/SOx 碳材料具有微/多孔结构,有利于电解质扩散,并通过法拉第氧化还原反应提高了速率能力和假电容。与已报道的生物质碳材料相比,N/SOx 碳材料具有显著的电容(1 Ag-1 时为 392 F g-1)和出色的循环稳定性(5000 次循环后保持率为 94.8%)。通过优化不同的壳聚糖质量比,使用木质素:壳聚糖样品比为 1:2 的对称超级电容器制备出了最有效的 N/SOx 炭材料 SNACM = S/N 掺杂活性炭材料(SNACM-2)。此外,基于 SNACM-2 的准固态对称超级电容器在 1 A g-1 时具有 142 F g-1 的出色比电容,同时还具有出色的柔韧性。在功率密度为 0.5 kW kg-1 时,SNACM-2 的能量密度高达 9.8 W h kg-1。这项研究提出了一种成功的策略,将低价值、生态友好型天然聚合物转化为可再生、高性能的超级电容器碳材料。
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引用次数: 0
Tissue-derived highly compressible anisotropic carbon aerogels with aligned fibrous matrices for solid-state rechargeable zinc-cobalt-air hybrid batteries 用于固态可充电锌-钴-空气混合电池的组织衍生型高可压缩各向异性碳气凝胶与排列整齐的纤维基质
Q1 CHEMISTRY, PHYSICAL Pub Date : 2023-12-12 DOI: 10.1002/eom2.12431
Ye-Eun Park, Seung-Hee Park, Sung Hoon Ahn

The rising demand for wearable zinc-air batteries encounters challenges in balancing electrochemical performance and mechanical resilience. Elastic carbon aerogels in air cathodes necessitate a metal content constraint of less than 3 wt.%, adversely impacting catalytic activity optimization. This study presents a novel fabrication method for fibrous carbon aerogels with high compressive resilience and extraordinary catalytic performance. An external layer of graphene shells and carbon nanotubes integrated onto the fibrous carbon matrix mitigates metallic species diffusion. This confinement ensures exceptional bi-catalytic activity for oxygen-involved redox reactions without compromising ultra-elasticity. With high cobalt content in the aerogel cathode, it exhibits minimal voltage gaps during charge–discharge cycles, showcasing unique zinc-cobalt-air hybrid battery characteristics. It sustains exceptional elasticity in repeated testing, achieving approximately 79.2% round-trip efficiency over a 60-h cycle test, underscoring its potential as a wearable energy storage device.

可穿戴锌-空气电池的需求不断增长,但在平衡电化学性能和机械弹性方面却遇到了挑战。空气阴极中的弹性碳气凝胶的金属含量必须小于 3 wt.%,这对催化活性的优化产生了不利影响。本研究提出了一种新颖的纤维状碳气凝胶制造方法,这种气凝胶具有很高的抗压回弹性和非凡的催化性能。在纤维状碳基质上集成了石墨烯壳和碳纳米管外层,可减轻金属物种的扩散。这种限制确保了在不影响超弹性的情况下,对与氧有关的氧化还原反应具有卓越的双催化活性。由于气凝胶阴极中的钴含量较高,因此在充放电循环过程中电压间隙极小,显示出独特的锌-钴-空气混合电池特性。它在反复测试中保持了超强的弹性,在 60 小时的循环测试中实现了约 79.2% 的往返效率,突出了其作为可穿戴储能设备的潜力。
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引用次数: 0
Photo-thermo-electric hydrogel with interlocking photothermal layer and hydrogel for enhancement of thermopower generation 具有互锁光热层和水凝胶的光热发电水凝胶,用于提高热发电量
Q1 CHEMISTRY, PHYSICAL Pub Date : 2023-12-10 DOI: 10.1002/eom2.12428
Jingjie Shen, Chenhui Yang, Yanli Ma, Mengnan Cao, Zifa Gao, Shuo Wang, Jian Li, Shouxin Liu, Zhijun Chen, Shujun Li

Photothermal devices and thermoelectric cells hold great promise for energy generation but integration of the two remains a considerable challenge in real-life power supply for sensors. Here, a novel photo-thermo-electric hydrogel (PTEH-Interlocking) was constructed by the synthesis of a photothermal layer on a thermoelectric hydrogel with the redox pair Fe(CN)63−/Fe(CN)64−. The smart design of using the oxidation of pyrogallic acid by Fe(CN)63− to construct the photothermal layer for photo-to-heat conversion protected the redox couple of the thermogalvanic ion pair from ultraviolet damage, as well as triggered the formation of an interlocking structure at the interface of the photothermal layer and the thermoelectric hydrogel. The as-prepared PTEH-Interlocking has shown a high Seebeck coefficient and rapid heat transfer, boosting the photo-thermo-electric conversion. As a demonstration of a practical application, the PTEH-Interlocking cells are successfully used as the energy supply for a mechanical sensor.

光热器件和热电电池在能源生产方面前景广阔,但在实际传感器供电方面,两者的整合仍是一个相当大的挑战。本文通过在热电水凝胶上合成光热层与氧化还原对 Fe(CN)63-/Fe(CN)64-,构建了一种新型光热电水凝胶(PTEH-Interlocking)。利用 Fe(CN)63- 氧化焦金酸来构建光热层进行光-热转换的巧妙设计保护了热电离子对的氧化还原对免受紫外线的破坏,并在光热层和热电水凝胶的界面上形成了互锁结构。制备的 PTEH-Interlocking 具有较高的塞贝克系数和快速传热的特性,从而促进了光热电转换。在实际应用中,PTEH 互锁电池被成功用作机械传感器的能源供应。
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引用次数: 0
NaGdF4:Yb,Er@ZIF-8/MnO2 for photocatalytic removal of organic pollutants and pathogenic bacteria NaGdF4:Yb,Er@ZIF-8/MnO2光催化去除有机污染物和致病菌
Q1 CHEMISTRY, PHYSICAL Pub Date : 2023-12-03 DOI: 10.1002/eom2.12427
Yue Shu, Yue Zhao, Xiaoyu Linghu, Wenqi Liu, Dan Shan, Changyuan Zhang, Ran Yi, Xiang Li, Baiqi Wang

In the field of environmental science, efficient removal of organic pollutants and pathogenic bacteria from wastewater using a photocatalytic process that responds to the full spectrum of sunlight is crucial. In this study, a highly effective nanoheterojunction called NaGdF4:Yb,Er@zeolitic imidazolate framework-8/manganese dioxide (NaGdF4:Yb,Er@ZIF-8/MnO2, UCZM) was synthesized. This nanoheterojunction exhibits a remarkable ability to respond to the entire range of ultraviolet, visible, and infrared light. Under simulated sunlight, UCZM demonstrated outstanding performance in degrading malachite green dye, with a degradation efficiency of 92.6% within 90 min. Moreover, UCZM completely inactivated both Staphylococcus aureus and Escherichia coli within 20 min under simulated sunlight. Mechanistic studies revealed that NaGdF4:Yb,Er played a crucial role in activating ZIF-8 and MnO2 through Förster resonance energy transfer, facilitating the photocatalytic process. The formation of a Z-type heterojunction in UCZM promoted the efficient separation of photogenerated carriers. Furthermore, UCZM exhibited excellent biosafety properties. This study represents the first exploration of a composite material composed of UCNPs, ZIF-8, and MnO2 for photocatalytic applications. The findings highlight the potential of this novel nanoheterojunction design, which exhibits a full spectral response, for tackling water pollution through efficient photocatalytic degradation of organic pollutants and inactivation of pathogenic bacteria.

在环境科学领域,利用响应全光谱阳光的光催化过程有效去除废水中的有机污染物和致病菌是至关重要的。在本研究中,合成了一种高效的纳米异质结,称为NaGdF4:Yb,Er@zeolitic咪唑酸骨架-8/二氧化锰(NaGdF4:Yb,Er@ZIF-8/MnO2, UCZM)。这种纳米异质结表现出对紫外光、可见光和红外光的全范围响应能力。在模拟阳光下,UCZM对孔雀石绿染料的降解性能优异,在90 min内降解效率达到92.6%。此外,UCZM在模拟阳光下20分钟内就能完全灭活金黄色葡萄球菌和大肠杆菌。机理研究表明,NaGdF4:Yb,Er通过Förster共振能量转移激活ZIF-8和MnO2,促进了光催化过程。UCZM中z型异质结的形成促进了光生载流子的有效分离。此外,UCZM还具有良好的生物安全性能。该研究首次探索了由UCNPs、ZIF-8和MnO2组成的光催化复合材料。这些发现突出了这种新型纳米异质结设计的潜力,它具有全光谱响应,可以通过有效的光催化降解有机污染物和灭活致病菌来解决水污染问题。
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引用次数: 0
Concave microlens arrays with tunable curvature for enhanced photodegradation of organic pollutants in water: A non-contact approach 具有可调曲率的凹微透镜阵列用于增强水中有机污染物的光降解:一种非接触方法
Q1 CHEMISTRY, PHYSICAL Pub Date : 2023-11-29 DOI: 10.1002/eom2.12426
Qiuyun Lu, Yanan Li, Kehinde Kassim, Ben Bin Xu, Mohamed Gamal El-Din, Xuehua Zhang

Solar-driven photodegradation for water treatment faces challenges such as low energy conversion rates, high maintenance costs, and over-sensitivity to the environment. In this study, we develop reusable concave microlens arrays (MLAs) for more efficient solar photodegradation by optimizing light distribution. Concave MLAs with the base radius of 5 μm are fabricated by imprinting convex MLAs to polydimethylsiloxane elastomers. Concave MLAs possess a non-contact reactor configuration, preventing MLAs from detaching or being contaminated. By precisely controlling the solvent exchange, concave MLAs are fabricated with well-defined curvature and adjustable volume on femtoliter scale. The focusing effects of MLAs are examined, and good agreement is presented between experiments and simulations. The photodegradation efficiency of organic pollutants in water is significantly enhanced by 5.1-fold, attributed to higher intensity at focal points of concave MLAs. Furthermore, enhanced photodegradation by concave MLAs is demonstrated under low light irradiation, applicable to real river water and highly turbid water.

太阳能驱动的光降解水处理面临着能量转化率低、维护成本高、对环境过于敏感等挑战。在这项研究中,我们开发了可重复使用的凹微透镜阵列(MLAs),通过优化光分布来提高太阳能光降解的效率。通过在聚二甲基硅氧烷弹性体上印迹制备了基底半径为~ 5 $$ sim 5 $$ μm的凹MLAs。凹mla具有非接触式反应器配置,防止mla分离或被污染。通过对溶剂交换的精确控制,制备出曲率明确、体积可调的飞升级凹面MLAs。实验结果与仿真结果吻合较好。由于凹形mla聚焦处的光强度更高,对水中有机污染物的光降解效率显著提高了5.1倍。此外,在弱光照射下,凹形MLAs增强了光降解,适用于真实河水和高浑浊水。
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