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An active learning workflow for predicting hydrogen atom adsorption energies on binary oxides based on local electronic transfer features 基于局部电子转移特征预测二元氧化物上氢原子吸附能的主动学习工作流程
IF 13.3 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-28 DOI: 10.1016/j.gee.2024.06.007
Wenhao Jing, Zihao Jiao, Mengmeng Song, Ya Liu, Liejin Guo
Machine learning combined with density functional theory (DFT) enables rapid exploration of catalyst descriptors space such as adsorption energy, facilitating rapid and effective catalyst screening. However, there is still a lack of models for predicting adsorption energies on oxides, due to the complexity of elemental species and the ambiguous coordination environment. This work proposes an active learning workflow (LeNN) founded on local electronic transfer features () and the principle of coordinate rotation invariance. By accurately characterizing the electron transfer to adsorption site atoms and their surrounding geometric structures, LeNN mitigates abrupt feature changes due to different element types and clarifies coordination environments. As a result, it enables the prediction of ∗H adsorption energy on binary oxide surfaces with a mean absolute error (MAE) below 0.18 eV. Moreover, we incorporate local coverage () and leverage neutral network ensemble to establish an active learning workflow, attaining a prediction MAE below 0.2 eV for 5419 multi-∗H adsorption structures. These findings validate the universality and capability of the proposed features in predicting ∗H adsorption energy on binary oxide surfaces.
机器学习与密度泛函理论(DFT)相结合,可以快速探索催化剂描述符空间(如吸附能),从而促进催化剂的快速有效筛选。然而,由于元素种类的复杂性和配位环境的模糊性,目前仍然缺乏预测氧化物吸附能的模型。本研究提出了一种基于局部电子转移特征()和坐标旋转不变性原理的主动学习工作流(LeNN)。通过准确描述电子传递到吸附位点原子及其周围几何结构的特征,LeNN 可减轻因元素类型不同而导致的特征突变,并澄清配位环境。因此,它能预测二元氧化物表面的 ∗H 吸附能,平均绝对误差 (MAE) 低于 0.18 eV。此外,我们还纳入了局部覆盖(),并利用中性网络集合建立了主动学习工作流程,使 5419 种多∗H 吸附结构的预测 MAE 低于 0.2 eV。这些发现验证了所提出的特征在预测二元氧化物表面∗H 吸附能方面的通用性和能力。
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引用次数: 0
2D/2D homojunction-mediated charge separation: Synergistic effect of crystalline C3N5 and g-C3N4 via electrostatic self-assembly for photocatalytic hydrogen and benzaldehyde production 二维/二维同质结介导的电荷分离:通过静电自组装实现晶体 C3N5 和 g-C3N4 在光催化制氢和苯甲醛生产中的协同效应
IF 13.3 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-06-27 DOI: 10.1016/j.gee.2024.06.008
Sue-Faye Ng, Joel Jie Foo, Peipei Zhang, Steven Hao Wan Kok, Lling-Lling Tan, Binghui Chen, Wee-Jun Ong
Homojunction engineering is a promising modification strategy to improve charge carrier separation and photocatalytic performance of carbon nitrides. Leveraging intrinsic heptazine/triazine phase and face-to-face contact, crystalline CN (CC3N5) was combined with protonated g-CN (pgCN) through electrostatic self-assembly to achieve robust 2D/2D homojunction interfaces. The highest photocatalytic performance was obtained through crystallinity and homojunction engineering, by controlling the pgCN:CC3N5 ratio. The 25:100 pgCN:CC3N5 homojunction (25CgCN) had the highest hydrogen production (1409.51 μmol h) and apparent quantum efficiency (25.04%, 420 nm), 8-fold and 180-fold higher than CC3N5 and pgCN, respectively. This photocatalytic homojunction improves benzaldehyde and hydrogen production activity, retaining 89% performance after 3 cycles (12 h) on a 3D-printed substrate. Electron paramagnetic resonance demonstrated higher ·OH, ·O and hole production of irradiated 25CgCN, attributed to crystallinity and homojunction interaction. Thus, electrostatic self-assembly to couple CC3N5 and pgCN in a 2D/2D homojunction interface ameliorates the performance of multifunctional solar-driven applications.
同质结工程是改善碳氮化物电荷载流子分离和光催化性能的一种前景广阔的改性策略。利用固有的庚嗪/三嗪相和面对面接触,通过静电自组装将结晶 CN(CC3N5)与质子化 g-CN(pgCN)结合在一起,实现了稳健的 2D/2D 同质结界面。通过控制 pgCN:CC3N5 的比例,结晶度和同结工程获得了最高的光催化性能。25:100 pgCN:CC3N5 同质结(25CgCN)的产氢量(1409.51 μmol h)和表观量子效率(25.04%,420 纳米)最高,分别比 CC3N5 和 pgCN 高 8 倍和 180 倍。这种光催化同质结提高了苯甲醛和氢气的生产活性,在三维打印基底上循环 3 次(12 小时)后,性能保持率仍高达 89%。电子顺磁共振显示,辐照 25CgCN 产生的-OH、-O 和空穴更多,这归因于结晶度和同质结的相互作用。因此,通过静电自组装将 CC3N5 和 pgCN 结合到二维/二维同质结界面中可改善多功能太阳能应用的性能。
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引用次数: 0
Research progress of lignin-derived materials in lithium/sodium ion batteries 锂离子/钠离子电池中木质素衍生材料的研究进展
IF 13.3 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-05-06 DOI: 10.1016/j.gee.2024.05.001
Jingke Zhang, Hengxue Xiang, Zhiwei Cao, Shichao Wang, Meifang Zhu
With the increase of energy consumption, the shortage of fossil resource, and the aggravation of environmental pollution, the development of cost-effective and environmental friendly bio-based energy storage devices has become an urgent need. As the second most abundant natural polymer found in nature, lignin is mainly produced as the by-product of paper pulping and bio-refining industries. It possesses several inherent advantages, such as low-cost, high carbon content, abundant functional groups, and bio-renewable, making it an attractive candidate for the rechargeable battery material. Consequently, there has been a surge of research interest in utilizing lignin or lignin-based carbon materials as the components of lithium-ion (LIBs) or sodium-ion batteries (SIBs), including the electrode, binder, separator, and electrolyte. This review provides a comprehensive overview on the research progress of lignin-derived materials used in LIBs/SIBs, especially the application of lignin-based carbons as the anodes of LIBs/SIBs. The preparation methods and properties of lignin-derived materials with different dimensions are systemically discussed, which emphasizes on the relationship between the chemical/physical structures of lignin-derived materials and the performances of LIBs/SIBs. The current challenges and future prospects of lignin-derived materials in energy storage devices are also proposed.
随着能源消耗的增加、化石资源的短缺和环境污染的加剧,开发经济、环保的生物基储能装置已成为当务之急。木质素是自然界中含量第二丰富的天然聚合物,主要产生于造纸制浆和生物精炼工业。木质素具有成本低、含碳量高、官能团丰富、生物可再生等固有优势,是一种极具吸引力的充电电池材料。因此,利用木质素或木质素基碳材料作为锂离子电池(LIBs)或钠离子电池(SIBs)的电极、粘结剂、隔膜和电解液等部件的研究兴趣日益高涨。本综述全面概述了木质素衍生材料用于锂离子电池/钠离子电池的研究进展,尤其是木质素基碳作为锂离子电池/钠离子电池阳极的应用。系统地讨论了不同维度木质素衍生材料的制备方法和性能,重点探讨了木质素衍生材料的化学/物理结构与 LIBs/SIBs 性能之间的关系。此外,还提出了木质素衍生材料在储能设备中的当前挑战和未来前景。
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引用次数: 0
CO2 electrolysis to formic acid for carbon neutralization 将二氧化碳电解为甲酸以实现碳中和
IF 13.3 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-05-04 DOI: 10.1016/j.gee.2024.04.011
Kezhen Qi, Shu-yuan Liu, Yingjie Zhang, Hui Zhang, Vadim Popkov, Oksana Almjasheva
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引用次数: 0
Facilitated transport membranes in post-combustion carbon capture: Recent advancements in polymer materials and challenges towards practical application 燃烧后碳捕获中的促进传输膜:聚合物材料的最新进展和实际应用面临的挑战
IF 13.3 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-04-29 DOI: 10.1016/j.gee.2024.04.010
Zihan Wang, Zhien Zhang, Mohamad Reza Soltanian, Ruizhi Pang
Facilitated transport membranes for post-combustion carbon capture are one of the technologies to achieve efficient and large-scale capture. The central principle is to utilize the affinity of CO for the carrier to achieve efficient separation and to break the Robson upper bound. This paper reviews the progress of facilitated transport membranes research regarding polymer materials, principles, and problems faced at this stage. Firstly, we briefly introduce the transport mechanism of the facilitated transport membranes. Then the research progress of several major polymers used for facilitated transport membranes for CO/N separation was presented in the past five years. Additionally, we analyze the primary challenges of facilitated transport membranes, including the influence of water, the effect of temperature, the saturation effect of the carrier, and the process configuration. Finally, we also delve into the challenges and competitiveness of facilitated transport membranes.
用于燃烧后碳捕集的促进传输膜是实现高效和大规模捕集的技术之一。其核心原理是利用一氧化碳对载体的亲和力实现高效分离,并打破罗布森上限。本文回顾了促进传输膜在聚合物材料、原理和现阶段面临的问题等方面的研究进展。首先,我们简要介绍了促进传输膜的传输机理。然后介绍了过去五年中用于 CO/N 分离的促进传输膜的几种主要聚合物的研究进展。此外,我们还分析了促进传输膜面临的主要挑战,包括水的影响、温度的影响、载体的饱和效应以及工艺配置。最后,我们还深入探讨了促进传输膜所面临的挑战和竞争力。
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引用次数: 0
Interfacial modulation of nano Li7La3Zr2O12 composite electrolytes prepared by solvent-free method 无溶剂法制备的纳米 Li7La3Zr2O12 复合电解质的界面调制
IF 13.3 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-04-27 DOI: 10.1016/j.gee.2024.04.009
Qigao Han, Yaqing Guo, Fuhe Wang, Xuechun Lou, Fengqian Wang, Jun Zhong, Jinqiao Du, Jie Tian, Weixin Zhang, Shun Tang, Shijie Cheng, Yuancheng Cao
Solid-state batteries (SSBs) with high safety are promising for the energy fields, but the development has long been limited by machinability and interfacial problems. Hence, supporting, Nano LLZO CSEs are prepared with a at . The contents of Nano LLZO particles enable the Nano LLZO CSEs to maintain good while exhibiting a wide electrochemical window of and a . The mean modulus reaches 4376 MPa. Benefiting from the , the Li|Li symmetric batteries based on the Nano LLZO CSEs show benign at the current densities of , , and . In addition, the Li|LiFePO (LFP) SSBs achieve favorable he specific capacity reaches at rate, with a capacity retention of about . In the further tests of the LiNiCoMnO (NCM811) cathodes with higher energy density, the Nano LLZO CSEs also demonstrate good compatibility: the specific capacities of NCM811-based SSBs reach at rate, while the capacity retention is over . Furthermore, the verify the and the potential for application, which have a desirable prospect.
具有高安全性的固态电池(SSBs)在能源领域大有可为,但其发展长期以来一直受到可加工性和界面问题的限制。因此,在纳米 LLZO CSEs 的制备过程中,需要在......的条件下进行支持。纳米 LLZO 颗粒的含量使纳米 LLZO CSEs 保持良好的电化学性能,同时显示出宽广的电化学窗口,其平均模量达到 4376 兆帕。此外,基于纳米 LLZO CSE 的锂-锂对称电池在电流密度为 、 、 和 时显示出良好的性能。 此外,锂-锂铁PO(LFP)SSB 的比容量达到了良好的速率,容量保持率约为 。在对能量密度更高的镍钴锰酸锂(NCM811)阴极的进一步测试中,纳米 LLZO CSE 也表现出良好的兼容性:基于 NCM811 的 SSB 的比容量达到率,而容量保持率超过 。此外,研究还验证了纳米 LLZO CSE 的性能和应用潜力,这些都具有令人向往的前景。
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引用次数: 0
Preparation and performance of highly-conductive dual-doped Li7La3Zr2O12 solid electrolytes for thermal batteries 用于热电池的高导电性双掺杂 Li7La3Zr2O12 固体电解质的制备及其性能
IF 13.3 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-04-11 DOI: 10.1016/j.gee.2024.04.002
Wei Li, Shu Zhang, Xinya Bu, Jing Luo, Yi Zhang, Mengyu Yan, Ting Quan, Yanli Zhu
Garnet LiLaZrO (LLZO) electrolytes have been recognized as a promising candidate to replace liquid/molten-state electrolytes in battery applications due to their exceptional performance, particularly Ga-doped LLZO (LLZGO), which exhibits high ionic conductivity. However, the limited size of the Li transport bottleneck restricts its high-current discharging performance. The present study focuses on the synthesis of Ga and Ba co-doped LLZO (LLZGBO) and investigates the influence of doping contents on the morphology, crystal structure, Li transport bottleneck size, and ionic conductivity. In particular, GaBa exhibits the highest ionic conductivity (6.11E-2 S cm at 550 °C) in comparison with other compositions, which can be attributed to its higher-energy morphology, larger bottleneck and unique Li transport channel. In addition to Ba, Sr and Ca have been co-doped with Ga into LLZO, respectively, to study the effect of doping ion radius on crystal structures and the properties of electrolytes. The characterization results demonstrate that the easier Li transport and higher ionic conductivity can be obtained when the electrolyte is doped with larger-radius ions. As a result, the assembled thermal battery with GaBa-LLZO electrolyte exhibits a remarkable voltage platform of 1.81 V and a high specific capacity of 455.65 mA h g at an elevated temperature of 525 °C. The discharge specific capacity of the thermal cell at 500 mA amounts to 63% of that at 100 mA, showcasing exceptional high-current discharging performance. When assembled as prototypes with fourteen single cells connected in series, the thermal batteries deliver an activation time of 38 ms and a discharge time of 32 s with the current density of 100 mA cm. These findings suggest that Ga, Ba co-doped LLZO solid-state electrolytes with high ionic conductivities holds great potential for high-capacity, quick-initiating and high-current discharging thermal batteries.
石榴石态 LiLaZrO(LLZO)电解质因其优异的性能,尤其是掺镓 LLZO(LLZGO)表现出的高离子电导率,已被公认为有望在电池应用中取代液态/熔融态电解质的候选材料。然而,锂传输瓶颈的有限尺寸限制了其大电流放电性能。本研究重点研究了镓和钡共掺杂 LLZO(LLZGBO)的合成,并考察了掺杂量对其形貌、晶体结构、锂传输瓶颈尺寸和离子电导率的影响。与其他成分相比,GaBa 尤其表现出最高的离子电导率(550 ℃ 时为 6.11E-2 S cm),这可归因于其较高能量的形貌、较大的瓶颈和独特的锂传输通道。除了 Ba 之外,LLZO 中还分别掺杂了 Sr 和 Ca,以研究掺杂离子半径对晶体结构和电解质性质的影响。表征结果表明,电解质中掺入较大半径的离子时,锂的传输更容易,离子电导率更高。因此,使用 GaBa-LLZO 电解质组装的热电池在 525 °C 的高温下显示出 1.81 V 的显著电压平台和 455.65 mA h g 的高比容量。热电池在 500 mA 时的放电比容量是 100 mA 时的 63%,显示出卓越的大电流放电性能。当把 14 个单体电池串联组装成原型时,热电池的激活时间为 38 毫秒,放电时间为 32 秒,电流密度为 100 毫安厘米。这些研究结果表明,具有高离子导电率的镓、钡共掺杂 LLZO 固态电解质在高容量、快速启动和大电流放电热电池方面具有巨大潜力。
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引用次数: 0
Energy transfer enhanced photocatalytic hydrogen evolution in organic heterostructure nanoparticles via flash nanoprecipitation processing 通过闪速纳米沉淀处理增强有机异质结构纳米粒子的能量转移光催化氢进化能力
IF 13.3 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-04-10 DOI: 10.1016/j.gee.2024.04.001
Miaojie Yu, Weiwei Zhang, Xueyan Liu, Guohui Zhao, Jun Du, Yongzhen Wu, Wei-Hong Zhu
Organic nanophotocatalysts are promising candidates for solar fuels production, but they still face the challenge of unfavorable geminate recombination due to the limited exciton diffusion lengths. Here, we introduce a binary nanophotocatalyst fabricated by blending two polymers, PS-PEG5 (PS) and PBT-PEG5 (PBT), with matched absorption and emission spectra, enabling a Förster resonance energy transfer (FRET) process for enhanced photocatalysis. These heterostructure nanophotocatalysts are processed using a facile and scalable flash nanoprecipitation (FNP) technique with precious kinetic control over binary nanoparticle formation. The resulting nanoparticles exhibits an exceptional photocatalytic hydrogen evolution rate up to 65 mmol g h, 2.5 times higher than that single component nanoparticle. Characterizations through fluorescence spectra and transient absorption spectra confirm the hetero-energy transfer within the binary nanoparticles, which prolongs the excited-state lifetime and extends the namely “effective exciton diffusion length”. Our finding opens new avenues for designing efficient organic photocatalysts by improving exciton migration.
有机纳米光催化剂是太阳能燃料生产的理想候选材料,但由于激子扩散长度有限,它们仍然面临着不利的宝石化重组挑战。在这里,我们介绍了一种二元纳米光催化剂,它是由两种聚合物(PS-PEG5(PS)和 PBT-PEG5(PBT))混合制成的,这两种聚合物的吸收光谱和发射光谱相匹配,从而实现了弗斯特共振能量转移(FRET)过程,增强了光催化功能。这些异质结构纳米光催化剂是利用一种简便、可扩展的闪速纳米沉淀(FNP)技术加工而成的,对二元纳米粒子的形成具有珍贵的动力学控制。所得到的纳米粒子具有优异的光催化氢进化率,高达 65 mmol g h,是单组分纳米粒子的 2.5 倍。通过荧光光谱和瞬态吸收光谱进行的表征证实了二元纳米粒子内部的异能传递,这延长了激发态的寿命,并延长了 "有效激子扩散长度"。我们的发现为通过改善激子迁移设计高效有机光催化剂开辟了新途径。
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引用次数: 0
Construction of an artificial zinc alloy layer toward stable zinc-metal anode 构建人工锌合金层,实现稳定的锌金属阳极
IF 13.3 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-04-04 DOI: 10.1016/j.gee.2024.03.006
Long Jiang, Yizhao Chai, Dongdong Ji, Liwei Li, Le Li, Bingan Lu, Dongmin Li, Jiang Zhou
Aqueous zinc-ion batteries (AZIBs) present a promising option for next-generation batteries given their high safety, eco-friendliness, and resource sustainability. Nonetheless, the practical application of zinc anodes is hindered by inevitable parasitic reactions and dendrite growth. Here, zinc alloy layers (i.e., ZnCo and ZnFe alloys) were rationally constructed on the zinc surface by chemical displacement reactions. The alloying process exposes more (002) planes of the ZnCo anode to guide the preferential and dendrite-free zinc deposition. Furthermore, the ZnCo alloy layer not only effectively inhibits water-induced side reactions but also accelerates electrode kinetics, enabling highly reversible zinc plating/stripping. As a result, the ZnCo anode achieves a Coulombic efficiency of 99.2% over 1300 cycles, and the ZnCo symmetric cell exhibits a long cycle life of over 2000 h at 4.4 mA cm. Importantly, the ZnCo//NHVO full cell retains a high discharge capacity of 218.4 mAh g after 800 cycles. Meanwhile, the ZnFe-based symmetric cell also displays excellent cycling stability over 2500 h at 1.77 mA cm. This strategy provides a facile anode modification approach toward high-performance AZIBs.
锌离子水电池(AZIBs)具有高度安全性、生态友好性和资源可持续性,是下一代电池的理想选择。然而,锌阳极的实际应用受到不可避免的寄生反应和枝晶生长的阻碍。在这里,我们通过化学置换反应在锌表面合理地构建了锌合金层(即锌钴合金和锌铁合金)。合金化过程暴露了锌钴阳极的更多 (002) 平面,从而引导了锌的优先和无枝晶沉积。此外,锌钴合金层不仅能有效抑制水引起的副反应,还能加速电极动力学,实现高度可逆的镀锌/剥离。因此,锌钴阳极在 1300 次循环中的库仑效率达到了 99.2%,锌钴对称电池在 4.4 mA cm 的条件下可实现超过 2000 小时的长循环寿命。重要的是,ZnCo//NHVO 全电池在 800 次循环后仍能保持 218.4 mAh g 的高放电容量。同时,基于锌钴的对称电池在 1.77 mA cm 的条件下也显示出了超过 2500 小时的卓越循环稳定性。这种策略为实现高性能 AZIB 提供了一种简便的阳极改性方法。
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引用次数: 0
Accelerating the practical application of MOFs for hydrogen storage—from performance-driven to application-oriented 加快 MOFs 在储氢领域的实际应用--从性能驱动到应用导向
IF 13.3 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-04-02 DOI: 10.1016/j.gee.2024.03.007
Yifan Wang, Jinghui Wu, Yidi Gao, Keqing Li, Chi Wang, Xiaochun Cui, Mingxin Huo, Xianze Wang
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引用次数: 0
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