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A Functional Cathode Sodium Compensation Agent for Stable Sodium-Ion Batteries 用于稳定钠离子电池的功能性阴极钠补偿剂
IF 13.3 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-03-02 DOI: 10.1016/j.gee.2024.02.009
Wei Wu, Zhenglin Hu, Zhengfei Zhao, Aoxuan Wang, Jiayan Luo
Hard carbon (HC) is widely used in sodium-ion batteries (SIBs), but its performance has always been limited by low initial Coulombic efficiency (ICE) and cycling stability. Cathode compensation agent is a favorable strategy to make up for the loss of active sodium ions consumed by HC anode. Yet it lacks agent that effectively decomposes to increase the active sodium ions as well as regulate carbon defects for decreasing the irreversible sodium ions consumption. Here, we propose 1,2-dihydroxybenzene Na salt (NaDB) as a cathode compensation agent with high specific capacity (347.9 mAh g), lower desodiation potential (2.4–2.8 V) and high utilization (99%). Meanwhile, its byproduct could functionalize HC with more CO groups and promotes its reversible capacity. Consequently, the presodiation hard carbon (pHC) anode exhibits highly reversible capacity of 204.7 mAh g with 98% retention at 5 C rate over 1000 cycles. Moreover, with 5 wt% NaDB initially coated on the NaV(PO) (NVP) cathode, the capacity retention of NVP + NaDB|HC cell could increase form 36%–89% after 1000 cycles at 1 C rate. This work provides a new avenue to improve SIBs reversible capacity and cycling performance through designing functional cathode compensation agent.
硬碳(HC)被广泛应用于钠离子电池(SIB),但其性能一直受到初始库仑效率(ICE)和循环稳定性较低的限制。阴极补偿剂是弥补碳氢化合物阳极消耗的活性钠离子损失的有利策略。然而,目前缺乏既能有效分解以增加活性钠离子,又能调节碳缺陷以减少不可逆钠离子消耗的药剂。在此,我们提出了 1,2-二羟基苯 Na 盐(NaDB)作为阴极补偿剂,它具有较高的比容量(347.9 mAh g)、较低的解碘电位(2.4-2.8 V)和较高的利用率(99%)。同时,其副产物可使碳氢化合物具有更多的 CO 基团,从而提高其可逆容量。因此,预阳极化硬碳(pHC)阳极在 5 C 速率下可在 1000 次循环中显示出 204.7 mAh g 的高可逆容量和 98% 的保持率。此外,在 NaV(PO)(NVP)阴极上涂覆 5 wt% 的 NaDB 后,NVP + NaDB|HC 电池在 1 C 速率下循环 1000 次后,容量保持率可提高 36%-89%。这项工作为通过设计功能性阴极补偿剂来提高 SIB 的可逆容量和循环性能提供了一条新途径。
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引用次数: 0
Organic Solvent Nanofiltration Membranes for Separation in Non-Polar Solvent System 用于非极性溶剂系统分离的有机溶剂纳滤膜
IF 13.3 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-02-29 DOI: 10.1016/j.gee.2024.02.007
Shuyun Gu, Siyao Li, Zhi Xu
Membrane technology holds significant potential for augmenting or partially substituting conventional separation techniques, such as heat-driven distillation, thereby reducing energy consumption. Organic solvent nanofiltration represents an advanced membrane separation technology capable of discerning molecules within a molecular weight range of approximately 100–1000 Da in organic solvents, offering low energy requirements and minimal carbon footprints. Molecular separation in non-polar solvent system, such as toluene, n-hexane, and n-heptane, has gained paramount importance due to their extensive use in the pharmaceutical, biochemical, and petrochemical industries. In this review, we presented recent advancements in membrane materials, membrane fabrication techniques and their promising applications for separation in non-polar solvent system, encompassing hydrocarbon separation, bioactive molecule purification and organic solvent recovery. Furthermore, this review highlighted the challenges and opportunities associated with membrane scale-up strategies and the direct translation of this promising technology into industrial applications.
膜技术在增强或部分替代传统分离技术(如热驱动蒸馏),从而降低能耗方面具有巨大潜力。有机溶剂纳滤是一种先进的膜分离技术,能够分辨有机溶剂中分子量范围约为 100-1000 Da 的分子,能耗低,碳足迹最小。由于甲苯、正己烷和正庚烷等非极性溶剂体系在制药、生化和石化工业中的广泛应用,这些溶剂体系中的分子分离已变得极为重要。在这篇综述中,我们介绍了膜材料、膜制造技术的最新进展及其在非极性溶剂系统中分离的应用前景,包括碳氢化合物分离、生物活性分子纯化和有机溶剂回收。此外,本综述还强调了与膜放大战略相关的挑战和机遇,以及将这一前景广阔的技术直接转化为工业应用的问题。
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引用次数: 0
Interfacial friction induced capillary flow within nanofiber-supported ionic liquid droplets 纳米纤维支撑的离子液体液滴内的界面摩擦诱导毛细流动
IF 13.3 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-02-28 DOI: 10.1016/j.gee.2024.02.008
Yuanyuan Zhao, Gang Xia, Yintung Lam, John Haozhong Xin
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引用次数: 0
Optimizing Electronic Structure through Point Defect Engineering for Enhanced Electrocatalytic Energy Conversion 通过点缺陷工程优化电子结构,提高电催化能量转换能力
IF 13.3 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-02-24 DOI: 10.1016/j.gee.2024.02.006
Wei Ma, Jiahao Yao, Fang Xie, Xinqi Wang, Hao Wan, Xiangjian Shen, Lili Zhang, Menggai Jiao, Zhen Zhou
Point defect engineering endows catalysts with novel physical and chemical properties, elevating their electrocatalytic efficiency. The introduction of defects emerges as a promising strategy, effectively modifying the electronic structure of active sites. This optimization influences the adsorption energy of intermediates, thereby mitigating reaction energy barriers, altering paths, enhancing selectivity, and ultimately improving the catalytic efficiency of electrocatalysts. To elucidate the impact of defects on the electrocatalytic process, we comprehensively outline the roles of various point defects, their synthetic methodologies, and characterization techniques. Importantly, we consolidate insights into the relationship between point defects and catalytic activity for hydrogen/oxygen evolution and CO/O/N reduction reactions by integrating mechanisms from diverse reactions. This underscores the pivotal role of point defects in enhancing catalytic performance. At last, the principal challenges and prospects associated with point defects in current electrocatalysts are proposed, emphasizing their role in advancing the efficiency of electrochemical energy storage and conversion materials.
点缺陷工程赋予催化剂新颖的物理和化学特性,从而提高其电催化效率。引入缺陷是一种很有前途的策略,可有效改变活性位点的电子结构。这种优化会影响中间产物的吸附能,从而减轻反应能量障碍、改变路径、提高选择性,并最终提高电催化剂的催化效率。为了阐明缺陷对电催化过程的影响,我们全面概述了各种点缺陷的作用、合成方法和表征技术。重要的是,我们通过整合不同反应的机理,对点缺陷与氢/氧进化和 CO/O/N 还原反应催化活性之间的关系进行了深入分析。这强调了点缺陷在提高催化性能方面的关键作用。最后,提出了当前电催化剂中与点缺陷相关的主要挑战和前景,强调了点缺陷在提高电化学储能和转换材料效率方面的作用。
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引用次数: 0
Recent advances of metal vacancies in energy and environmental catalysis: synthesis, characterization, and roles 金属空位在能源和环境催化方面的最新进展:合成、表征和作用
IF 13.3 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-02-22 DOI: 10.1016/j.gee.2024.02.005
Long Sun, Shunzheng Zhao, Sirui Gao, Ronghui Zhu, Yiran Tan, Xiaolong Tang, Honghong Yi
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引用次数: 0
Atmospheric reductive catalytic fractionation of lignocellulose integrated with one-pot catalytic conversion of carbohydrate yielding valuable lignin monomers and platform chemicals from corn straw 木质纤维素的常压还原催化分馏与碳水化合物的一次性催化转化相结合,从玉米秸秆中获得有价值的木质素单体和平台化学品
IF 13.3 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-02-21 DOI: 10.1016/j.gee.2024.02.004
Meng-Ying Liu, Zhe-Hui Zhang, Xue-Qi Wang, Qian Sun, Chen Zhang, Yu Li, Zhuohua Sun, Katalin Barta, Feng Peng, Tong-Qi Yuan
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引用次数: 0
Direct seawaect seawter splitting for hydrogen production: recent advances in materials synthesis and technological innovation 直接海水分离制氢:材料合成和技术创新的最新进展
IF 13.3 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-02-03 DOI: 10.1016/j.gee.2024.02.001
Yilin Zhao, Zhipeng Yu, Aimin Ge, Lujia Liu, Joaquim Luis Faria, Guiyin Xu, Meifang Zhu

Direct seawater splitting has emerged as a popular and promising research direction for the synthesis of clean, green, non-polluting, and sustainable hydrogen energy without depending on high-purity water in the face of the world's shortage of fossil energy. However, efficient seawater splitting is hindered by slow kinetics caused by the ultra-low conductivity and the presence of bacteria, microorganisms, and stray ions in seawater. Additionally, producing hydrogen on an industrial scale is challenging due to the high production cost. To address these challenges, this review presents that from the catalyst point of view, designing catalysts with high catalytic activity and high stability can directly affect the rate and effect of seawater splitting. From the ion transfer perspective, designing membranes can block harmful ions, improving the stability of seawater splitting. From the energy point of view, mixed seawater systems and self-powered systems also provide new and low-energy research systems for seawater splitting. Finally, ideas and directions for further research on direct seawater splitting in the future are pointed out, with the aims of achieving low-cost and high-efficiency hydrogen production.

在全球化石能源短缺的情况下,直接海水裂解已成为无需依赖高纯度水即可合成清洁、绿色、无污染和可持续氢能源的一个热门且前景广阔的研究方向。然而,海水的超低电导率以及海水中细菌、微生物和杂散离子的存在导致的缓慢动力学阻碍了海水的高效分裂。此外,由于生产成本高昂,在工业规模上生产氢气具有挑战性。为应对这些挑战,本综述指出,从催化剂的角度来看,设计具有高催化活性和高稳定性的催化剂可直接影响海水裂解的速率和效果。从离子传输的角度来看,设计膜可以阻挡有害离子,提高海水裂解的稳定性。从能源角度看,混合海水系统和自供电系统也为海水分质提供了新的低能耗研究系统。最后,指出了未来进一步研究海水直接裂解的思路和方向,以期实现低成本、高效率的制氢。
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引用次数: 0
High-throughput screening of CO2 cycloaddition MOF catalyst with an explainable machine learning model 利用可解释的机器学习模型高通量筛选 CO2 环加成 MOF 催化剂
IF 13.3 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-02-03 DOI: 10.1016/j.gee.2024.01.010
Xuefeng Bai, Yi Li, Yabo Xie, Qiancheng Chen, Xin Zhang, Jian-Rong Li

The high porosity and tunable chemical functionality of metal-organic frameworks (MOFs) make it a promising catalyst design platform. High-throughput screening of catalytic performance is feasible since the large MOF structure database is available. In this study, we report a machine learning model for high-throughput screening of MOF catalysts for the CO2 cycloaddition reaction. The descriptors for model training were judiciously chosen according to the reaction mechanism, which leads to high accuracy up to 97% for the 75% quantile of the training set as the classification criterion. The feature contribution was further evaluated with SHAP and PDP analysis to provide a certain physical understanding. 12,415 hypothetical MOF structures and 100 reported MOFs were evaluated under 100 °C and 1 bar within one day using the model, and 239 potentially efficient catalysts were discovered. Among them, MOF-76(Y) achieved the top performance experimentally among reported MOFs, in good agreement with the prediction.

金属有机框架(MOFs)的高孔隙率和可调化学功能使其成为一种前景广阔的催化剂设计平台。由于拥有庞大的 MOF 结构数据库,因此对催化性能进行高通量筛选是可行的。在本研究中,我们报告了一种用于高通量筛选 CO2 环加成反应 MOF 催化剂的机器学习模型。我们根据反应机理明智地选择了用于模型训练的描述符,这使得以训练集的 75% 四分位数作为分类标准的准确率高达 97%。通过 SHAP 和 PDP 分析进一步评估了特征贡献,以提供一定的物理理解。利用该模型在一天之内对 12,415 种假设的 MOF 结构和 100 种已报道的 MOF 在 100 °C 和 1 bar 下进行了评估,发现了 239 种潜在的高效催化剂。其中,MOF-76(Y) 的实验性能在已报道的 MOF 中名列前茅,与预测结果非常吻合。
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引用次数: 0
CoTCPP integrates with BiOBr microspheres for improved solar-driven CO2 reduction performance CoTCPP 与 BiOBr 微球相结合,提高了太阳能驱动的二氧化碳减排性能
IF 13.3 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-02-01 DOI: 10.1016/j.gee.2024.01.008
Lina Li, Yi Zhang, Gaopeng Liu, Tiange Wei, Junze Zhao, Bin Wang, Mengxia Ji, Yuanbin She, Jiexiang Xia, Huaming Li

CO2 photoreduction into carbon-based chemicals has been considered as an appropriate way to alleviate the energy issue and greenhouse effect. Herein, the 5, 10, 15, 20-tetra (4-carboxyphenyl) porphyrin cobalt(II) (CoTCPP) has been integrated with BiOBr microspheres and formed the CoTCPP/BiOBr composite. The as-prepared CoTCPP/BiOBr-2 shows optimized photocatalytic performance for CO2 conversion into CO and CH4 upon irradiation with 300 W Xe lamp, which is 2.03 and 2.58 times compared to that of BiOBr, respectively. The introduced CoTCPP significantly enhanced light absorption properties, promoted rapid separation of photogenerated carriers and boosted the chemisorption of CO2 molecules. The metal Co2+ at the center of the porphyrin molecules also acts as adsorption center for CO2 molecules, boosting the CO2 convert into CO and CH4. The possible mechanism of CO2 photoreduction was explored by in-situ FT-IR spectra. This work offers a new possibility for the preparation of advance photocatalysts.

将二氧化碳光降解为碳基化学品被认为是缓解能源问题和温室效应的适当途径。本文将 5、10、15、20-四(4-羧基苯基)卟啉钴(II)(CoTCPP)与 BiOBr 微球结合,形成 CoTCPP/BiOBr 复合材料。制备的 CoTCPP/BiOBr-2 在 300 W Xe 灯照射下,将 CO2 转化为 CO 和 CH4 的光催化性能达到最佳,分别是 BiOBr 的 2.03 倍和 2.58 倍。引入的 CoTCPP 显著增强了光吸收性能,促进了光生载流子的快速分离,并提高了 CO2 分子的化学吸附能力。卟啉分子中心的金属 Co2+ 也成为 CO2 分子的吸附中心,促进 CO2 转化为 CO 和 CH4。通过原位傅立叶变换红外光谱,探索了二氧化碳光生化的可能机制。这项工作为制备先进的光催化剂提供了新的可能性。
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引用次数: 0
Industrial solid wastes to environmental protection materials for removal of gaseous pollutants: A review 将工业固体废物转化为去除气态污染物的环保材料:综述
IF 13.3 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-01-25 DOI: 10.1016/j.gee.2024.01.006
Jiacheng Bao, Xin Sun, Ping Ning, Kai Li, Jie Yang, Fei Wang, Lei Shi, Maohong Fan

The application of industrial solid wastes as environmentally functional materials for air pollutants control has gained much attention in recent years due to its potential to reduce air pollution in a cost-effective manner. In this review, we investigate the development of industrial-waste-based functional materials for various gas pollutant removal and consider the relevant reaction mechanism according to different types of industrial solid waste. We see a recent effort towards achieving high-performance environmental functional materials via chemical or physical modification, in which the active components, pore size, and phase structure can be altered. The review will discuss the potential of using industrial solid wastes, these modified materials, or synthesized materials from raw waste precursors for the removal of air pollutants, including SO2, NOx, Hg0, H2S, VOCs, and CO2. The challenges still need to be addressed to realize this potential and the prospects for future research fully. The suggests for future directions include determining the optimal composition of these materials, calculating the real reaction rate and turnover frequency, developing effective treatment methods, and establishing chemical component databases of raw industrial solid waste for catalysts/adsorbent preparation.

近年来,工业固体废物作为环境功能材料在大气污染物控制方面的应用备受关注,因为它具有以经济有效的方式减少大气污染的潜力。在这篇综述中,我们研究了基于工业废物的功能材料在去除各种气体污染物方面的发展,并根据不同类型的工业固体废物考虑了相关的反应机理。我们看到了近年来通过化学或物理改性实现高性能环保功能材料的努力,其中的活性成分、孔径和相结构都可以改变。本综述将讨论利用工业固体废物、这些改性材料或从原始废物前体中合成的材料去除空气污染物(包括二氧化硫、氮氧化物、氧化汞、硫化氢、挥发性有机化合物和二氧化碳)的潜力。要充分实现这一潜力和未来研究前景,仍需应对各种挑战。对未来方向的建议包括确定这些材料的最佳成分、计算实际反应速率和周转频率、开发有效的处理方法,以及建立用于催化剂/吸附剂制备的原始工业固体废物化学成分数据库。
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引用次数: 0
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Green Energy & Environment
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