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An overview of various critical aspects of low-cobalt/cobalt-free Li-ion battery cathodes
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-12-10 DOI: 10.1039/D4SE01206B
Sourav Mallick, Arjun Patel, Mariappan Parans Paranthaman, Jethrine H. Mugumya, Sunuk Kim, Michael L. Rasche, Mo Jiang, Herman Lopez and Ram B. Gupta

Cathodes of lithium-ion batteries (LIBs) significantly impact the environmental footprint, cost, and energy performance of the battery-pack. Hence, sustainable production of Li-ion battery cathodes is critically required for ensuring cost-effectiveness, environmental benignity, consumer friendliness, and social justice. Battery chemistry largely determines individual cell performance as well as the battery pack cost and life cycle greenhouse gas emission. Continuous manufacturing platforms improve production efficiency in terms of product yield, quality and cost. Spent-battery recycling ensures the circular economy of critical elements that are required for cathode production. Innovations in fast-charging LIBs are particularly promising for sustainable e-mobility with a reduced carbon footprint. This article provides an overview of these research directions, emphasizing strategies for low-cobalt cathode development, recycling processes, continuous production and improvement in fast-charging capability.

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引用次数: 0
Thermogalvanic bricks: optimising large dimension thermocells for air and water valorisation†
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-12-10 DOI: 10.1039/D4SE01498G
Rebecca Haughton-James, Sireenya Mesawang, Mark A. Buckingham, Robert Taylor, Patrick E. Phelan and Leigh Aldous

Thermogalvanic cells can potentially valorise the huge quantity of energy available as waste heat; using entropy-driven thermoelectrochemistry they can convert a thermal gradient into electricity. Most investigations exploit a thermal source (e.g. hot water, the human body, sunlight, electronics) via a heat exchanger (metal pipe, skin, housing, etc), combined with an unlimited heat sink (e.g. pumped cold water). Limited studies have used ambient air as the heat sink. This study is believed to be the first to explore using air as both the thermal source and heat sink. It compares thermogalvanic cell performance when using water–water and air–air as the thermal energy sources and sinks, respectively, for devices with relatively large physical dimensions (25 to 100 mm wide). Gelation improved power output under both scenarios, due to enhanced thermal isolation of the electrodes; power decreased with increasing width in the water–water setup, but power increased with increasing width for air–air harvesting. Water–water yielded higher power overall, yet the air–air system operated passively and could be further optimised for real-world applications, i.e. as thermogalvanic bricks or panels in building materials.

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引用次数: 0
Benzobisthiazole covalent organic framework photocatalysis for selective oxidation of benzyl amines† 苯并双噻唑共价有机框架光催化选择性氧化苯并胺†
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-12-09 DOI: 10.1039/D4SE01634C
Shengquan Zhu, Hongxiang Zhao, Yuexin Wang, Zheng Li, Siyu Zhang, Bing Zeng, Xue Zhou, Xiang-Kui Gu and Xianjun Lang

Covalent organic frameworks (COFs) enable highly effective photocatalysis due to their crystallinity, tunable pores and channels, and expansive light absorption. The performance of COFs in photocatalysis is underpinned by the intrinsic tendency of charge separation and transfer, thereby depending on the molecular building blocks. Benzobisthiazole (BBT), with an electron-withdrawing effect, shows superior potential in various optoelectronic materials. Therefore, with tetrabutylammonium hydroxide as a catalyst, a fully conjugated COF, BBT-sp2c-COF, is synthesized from 2,2′-(benzo[1,2-d:4,5-d′]bis(thiazole)-2,6-diyl)diacetonitrile and 1,3,6,8-tetrakis(4-formylphenyl)pyrene. As such, a series of characterizations demonstrate the structural and optical properties of BBT-sp2c-COF. The fully conjugated COF, BBT-sp2c-COF, possesses enhanced charge separation, electron transfer, and recycling stability. As expected, BBT-sp2c-COF photocatalysis achieves effective selective oxidation of benzyl amines with oxygen under blue light irradiation. Superoxide is identified as the crucial reactive oxygen species during the formation of imines. The full conjugation of organic building blocks into COFs can achieve highly effective photocatalysis.

共价有机框架(COFs)由于其结晶性、可调节的孔和通道以及广泛的光吸收而具有高效的光催化作用。COFs在光催化中的性能是由电荷分离和转移的内在趋势所支撑的,因此取决于分子构建块。苯并双噻唑(BBT)具有吸电子效应,在各种光电材料中表现出优异的潜力。因此,以四丁基氢氧化铵为催化剂,以2,2 ' -(苯并[1,2-d:4,5-d ']二(噻唑)-2,6-二基)二乙腈和1,3,6,8-四(4-甲基苯基)芘为原料合成了全共轭COF BBT-sp2c-COF。因此,一系列表征证明了BBT-sp2c-COF的结构和光学性质。完全共轭COF, BBT-sp2c-COF,具有更强的电荷分离、电子转移和循环稳定性。正如预期的那样,BBT-sp2c-COF光催化在蓝光照射下实现了苯胺与氧的有效选择性氧化。超氧化物被认为是亚胺形成过程中至关重要的活性氧。有机构建块与COFs的完全共轭可以实现高效的光催化。
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引用次数: 0
Life cycle assessment of plasma gasification integrated molten carbonate fuel cells and chemical looping reforming using RDF feedstock 使用RDF原料的等离子气化集成熔融碳酸盐燃料电池和化学循环重整的生命周期评估
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-12-09 DOI: 10.1039/D4SE01338G
Roni Mallick and Prabu Vairakannu

Refused derived fuel (RDF) is finding suitable applications in thermochemical conversion methods, including plasma gasification, to generate clean syngas. This addresses both the challenges of sustainable energy and waste management. In this study, RDF waste is utilized in a plasma gasification unit integrated with combined cycle, molten carbonate fuel cell (IPGCC-MCFC) and chemical looping reforming (IPGCC-CLR) systems for the co-generation of hydrogen and electricity. The simulations of the proposed plants are conducted using Aspen Plus software, and subsequently, the techno-economic assessment and life cycle analysis are performed. The results indicated that the highest net overall energy efficiency of 66.05%, lowest cost of electricity of 74.90 $ per MW h and levelized cost of hydrogen of 1.02 $ per kg, can be obtained for the IPGCC-CLR system. This improved the energy return on investment to 2.89 MW/MW as compared to 1.69 MW/MW for the IPGCC-MCFC plant. The life cycle analysis estimated the total fossil fuel consumption of 5.06–6.16 MJ s−1 and CO2 emissions of 285.14–335.61 gCO2eq. s−1 throughout the project duration. The plants reduce fossil fuel consumption by 1.5 times and CO2 emissions by 3 times as compared to the reported literature. Moreover, the analyses of other factors of environmental impact types of acidification potential, eutrophication potential, human toxicity potential, etc., show that the RDF processing stage contributes the largest pollution, followed by hydrogen compression and the transportation stage. The emissions can be minimized by replacing fossil fuels with hydrogen-based products at every stage.

拒绝衍生燃料(RDF)正在寻找合适的应用于热化学转化方法,包括等离子气化,以产生清洁的合成气。这既解决了可持续能源的挑战,也解决了废物管理的挑战。在这项研究中,RDF废物被用于等离子气化装置,该装置与联合循环、熔融碳酸盐燃料电池(ipgc - mcfc)和化学环重整(ipgc - clr)系统相结合,用于氢气和电力的热电联产。利用Aspen Plus软件对拟建电厂进行了模拟,并进行了技术经济评价和生命周期分析。结果表明,ipgc - clr系统的最高净总能源效率为66.05%,最低电力成本为74.90美元/ MW h,氢气平准化成本为1.02美元/ kg。与ipgc - mcfc电厂的1.69 MW/MW相比,这将能源投资回报率提高到2.89 MW/MW。生命周期分析估计化石燃料总消耗量为5.06-6.16 MJ s−1,CO2排放量为285.14-335.61 gCO2eq。S−1。与文献报道相比,这些植物减少了1.5倍的化石燃料消耗和3倍的二氧化碳排放。此外,对酸化潜力、富营养化潜力、人体毒性潜力等其他环境影响类型因素的分析表明,RDF加工阶段的污染贡献最大,其次是氢气压缩和运输阶段。通过在每个阶段用氢基产品取代化石燃料,可以最大限度地减少排放。
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引用次数: 0
Coal gasification slag-based-sodium acetate trihydrate composite phase change materials for solar thermal energy storage 煤气化炉渣-三水合乙酸钠复合相变材料用于太阳能热储能
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-12-06 DOI: 10.1039/D4SE00844H
Yawen Zhang, Minghao Fang, Xin Li, Zongce Chai, Zijiao Guo and Xin Min

Sodium acetate trihydrate (SAT) is an extremely potential low-temperature phase change material (PCM) in the solar power absorption, residual heat recovery, and other fields. Using coal gasification slag as a matrix for the sorption of SAT not only effectively solves the liquid leakage problem that occurs when the material is transferred from the solid phase to the liquid phase and but also improve the photothermal performance of the PCM, which is both environmentally friendly and economically valuable. A shape-stabilized coal gasification slag/sodium acetate trihydrate composite phase change material was therefore created in this work using the vacuum impregnation process, and its characteristics were examined. It was found that CGS is chemically compatible with SAT, and a CGS loading on SAT is 67.99%. on SAT results in a CPCM with better heat stability. Furthermore, the CPCM's latent heat could reach up to 171 J g−1, and it exhibited excellent capability for solar thermal conversion, with an photothermal conversion efficiency of 77.8%.

三水合乙酸钠(SAT)是一种在太阳能吸收、余热回收等领域极具潜力的低温相变材料。利用煤气化渣作为基体吸附SAT,不仅有效解决了材料从固相转移到液相时发生的漏液问题,而且提高了PCM的光热性能,既环保又经济。采用真空浸渍法制备了形状稳定的煤气化渣/三水合乙酸钠复合相变材料,并对其性能进行了研究。结果表明,CGS与SAT具有良好的化学相容性,CGS在SAT上的负载量为67.99%。在SAT上得到的CPCM具有更好的热稳定性。CPCM的潜热可达171 J g−1,具有良好的光热转换能力,光热转换效率达77.8%。
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引用次数: 0
Construction of a cross-linked network structure for a super-stable and long-life ZnO anode† 超稳定长寿命氧化锌阳极交联网络结构的构建
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-12-05 DOI: 10.1039/D4SE01288G
Zibo Chen, Ziyuan Wang, Zheng Li, Hao Cheng, Yao Lu, Chao Chen, Xingyi Li, Hailin Yu, Zhongliang Tian and Ke Peng

For alkaline zinc secondary batteries, the hydrogen evolution corrosion and dendrite growth on the zinc anode result in its short cycle life and low capacity. Currently, the occurrence of side reactions is inhibited by anode alloyage, electrode or electrolyte additives, or altering the structural design of the electrode. Among them, altering the structural design can effectively enhance the cycling performance. Furthermore, the 3D interconnected network structure can realize a uniform electric field and ion distribution to improve the electrode reaction behavior. Inspired by this, a ZnO anode with a 3D cross-linked network structure was constructed using CNFs as the 3D skeleton. By regulating the ZnO content and the ratio of CNFs/CB in the ZnO@CNFs/CB materials, the effect of the component content on the performance of the ZnO anodes was analyzed. With the increase in ZnO contents and CNFs/CN ratios, the reversibility, hydrogenation inhibition effect, cycling performance and rate performance of the ZnO anodes first showed an increasing trend, followed by a decreasing trend. When the theoretical mass ratio (ZnO : CNFs : CB) between the components in the ZnO@CNFs/CB material was 8 : 1 : 1, it exhibited a high hydrogenation inhibition effect and reversibility. When the prepared materials were used as the ZnO anode material of the zinc–nickel battery, the specific discharge capacity after 600 cycles at 1C rate was 566.90 mA h g−1, the coulombic efficiency was 86.02%, and the capacity retention rate was 90.17%. The average specific discharge capacity was 602.66 mA h g−1.

对于碱性锌二次电池,锌阳极的析氢腐蚀和枝晶生长导致其循环寿命短,容量低。目前,副反应的发生主要通过阳极合金、电极或电解质添加剂或改变电极的结构设计来抑制。其中,改变结构设计可以有效提高循环性能。此外,三维互连的网络结构可以实现均匀的电场和离子分布,从而改善电极的反应行为。受此启发,以CNFs为三维骨架,构建了具有三维交联网络结构的ZnO阳极。通过调节ZnO@CNFs/CB材料中ZnO的含量和CNFs/CB的比例,分析了组分含量对ZnO阳极性能的影响。随着ZnO含量和CNFs/CN比的增加,ZnO阳极的可逆性、氢化抑制效果、循环性能和速率性能均呈现先增加后降低的趋势。当ZnO@CNFs/CB材料中各组分的理论质量比(ZnO: CNFs: CB)为8:1:1时,表现出较高的加氢抑制效果和可逆性。当所制备的材料作为锌镍电池的ZnO负极材料时,在1C倍率下循环600次后的比放电容量为566.90 mA h g−1,库仑效率为86.02%,容量保持率为90.17%。平均比放电容量为602.66 mA h g−1。
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引用次数: 0
Manganese anodes for neutral electrolyte primary metal–air batteries†
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-12-05 DOI: 10.1039/D4SE01413H
Quinik L. Reyes-Morales, J. Rene Rangel-Mendez and Luis F. Chazaro-Ruiz

This study presents the first application of metallic manganese as an anode in metal–air batteries, to the best of our knowledge, achieving an energy density of 1859 W h kg−1 and a specific capacity of 1930 A h kg−1 through galvanostatic discharge tests. This system delivers 2.5 times more energy per gram than zinc, a commonly used metal in metal–air batteries, under identical testing conditions. Electrochemical analysis and discharge by-product studies revealed a discharge process through three oxidation states of manganese: Mn, Mn(II), and Mn(III). The combined attributes of manganese, including its abundance and environmental stability, position the Mn–air battery as a viable and sustainable option for energy storage from intermittent renewable sources.

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引用次数: 0
Efficient cascade conversion of glucose to levulinic acid using a dual-functional UiO-66 catalyst† 双功能UiO-66催化剂对葡萄糖级联转化为乙酰丙酸的研究
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-12-02 DOI: 10.1039/D4SE01352B
Sininat Boonmark, Panyapat Ponchai, Kanyaporn Adpakpang, Taya Saothayanun, Yollada Inchongkol, Natchaya Phongsuk and Sareeya Bureekaew

The catalytic properties of UiO-66 were enhanced through a post-synthetic defect engineering method. This involved facile treatment of the material with aqueous HCl to induce defects that generated free carboxylic acid (–COOH) groups. Consequently, the modified UiO-66 framework incorporated both Brønsted acidic –COOH groups and Lewis acidic sites, which originate from inherent linker-missing defects. These dual-functional acidic sites, combined with the high structural stability of UiO-66, enable it to act as an efficient heterogeneous catalyst for one-pot, multistep reactions. Specifically, the catalyst facilitates the conversion of glucose to levulinic acid (LEV) in the presence of sodium chloride (NaCl) as a promoter under hydrothermal conditions. Under optimized conditions (190 °C for 6 h), the catalytic system achieves a remarkable conversion of glucose (>99%), with an impressive 83% yield of LEV. The defect-engineered UiO-66 catalyst shows exceptional potential as a candidate for sugar conversion to valuable bio-based chemicals.

通过合成后缺陷工程方法提高了UiO-66的催化性能。这包括用盐酸水溶液对材料进行简单处理,以诱导产生游离羧酸(-COOH)基团的缺陷。因此,修改后的UiO-66框架包含了Brønsted酸性-COOH基团和Lewis酸性位点,这是由于固有的连接缺失缺陷造成的。这些双功能酸性位点,加上UiO-66的高结构稳定性,使其能够作为一锅多步骤反应的高效非均相催化剂。具体来说,在水热条件下,在氯化钠(NaCl)作为促进剂存在的情况下,该催化剂促进葡萄糖转化为乙酰丙酸(LEV)。在优化的条件下(190°C 6 h),催化系统实现了显著的葡萄糖转化率(>99%), LEV的收率达到了令人印象深刻的83%。缺陷工程的UiO-66催化剂作为糖转化为有价值的生物基化学品的候选物显示出非凡的潜力。
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引用次数: 0
Light-intensity dependence of visible-light CO2 reduction over Ru(ii)-complex/Ag/polymeric carbon nitride hybrid photocatalysts†
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-12-02 DOI: 10.1039/D4SE01488J
Ryuichi Nakada, Chao Zhang, Jo Onodera, Toshiya Tanaka, Megumi Okazaki, Guigang Zhang and Kazuhiko Maeda

Photocatalytic CO2 reduction over Ru(II)-complex/Ag/polymeric carbon nitride (PCN) was studied with respect to light intensity and the type of Ru(II) complex. In experiments using two different Ru(II) complex cocatalysts, the reduction potential of the Ru complex was found to balance efficient CO2 reduction on the Ru complex with electron transfer from Ag/PCN. This balance avoided the formation of H2 as a byproduct, minimized charge accumulation in Ag/PCN, and maximized the apparent quantum yield for CO2-to-HCOOH conversion.

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引用次数: 0
Interfacial engineering of a bifunctional electrocatalyst with outstanding catalytic performance, high intrinsic activity and solar-to-hydrogen conversion efficiency† 具有优异催化性能、高本征活性和太阳能-氢转化效率的双功能电催化剂的界面工程
IF 5 3区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2024-11-29 DOI: 10.1039/D4SE01320D
Muthukumaran Sangamithirai, Murugan Vijayarangan, Murugan Muthamildevi, Venkatachalam Ashok and Jayaraman Jayabharathi

Carbides are commonly regarded as efficient hydrogen evolution reaction (HER) catalysts, but their poor oxygen evolution reaction (OER) catalytic activities seriously limit their practical application in overall water splitting. Herein, embedded nanosheets and plates of cobalt oxy carbide (Co–O–C/CPs) were successfully synthesized as an efficient bifunctional electrocatalyst using a solvent-free combustion process. To contribute to the clarification of catalytic particle composition during electrochemical reactions, we thoroughly characterized the Co–O–C/CPs using HR-TEM, which revealed that the filled nanoplates, with a cobalt oxide shell and cobalt carbide core, were wrapped with carbon. During electrochemical reactions, the filled nanoplates changed to an amorphous state owing to the decomposition of the crystalline material. After amorphization, the Co–O–C/CPs maintained the shape of the parent compound and exhibited a higher electrochemically active surface area (ECSA) and thereby demonstrated enhanced HER (115 mV) and OER (240 mV) performances at 10 mA cm−2. When applying the Co–O–C/CPs as both the cathode and anode, a lower cell voltage of 1.60 V was required at 10 mA cm−2 than that for the benchmark catalyst IrO2/Pt/C/NF (1.63 V) with great stability in alkaline solution. This work provides a feasible strategy to fabricate cobalt oxy carbides and explores their possibility as bifunctional catalysts for water splitting.

碳化物通常被认为是高效的析氢反应(HER)催化剂,但其较差的析氧反应(OER)催化活性严重限制了其在整体水裂解中的实际应用。本文采用无溶剂燃烧方法,成功地合成了碳化钴氧纳米片和纳米板(Co-O-C /CPs)作为高效双功能电催化剂。为了澄清电化学反应过程中催化颗粒的组成,我们使用HR-TEM对Co-O-C /CPs进行了全面表征,结果表明,填充的纳米板具有氧化钴外壳和碳化钴芯,并被碳包裹。在电化学反应过程中,由于晶体材料的分解,填充的纳米板变为非晶态。非晶化后,Co-O-C /CPs保持了母体化合物的形状,并表现出更高的电化学活性表面积(ECSA),从而在10 mA cm−2下表现出更高的HER (115 mV)和OER (240 mV)性能。当Co-O-C /CPs同时作为阴极和阳极时,电池电压在10 mA cm - 2时为1.60 V,比基准催化剂IrO2/Pt/C/NF (1.63 V)低,且在碱性溶液中稳定性好。本研究为钴氧碳化物的制备提供了一种可行的策略,并探索了其作为水裂解双功能催化剂的可能性。
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引用次数: 0
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