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Enhanced charge storage in supercapacitors using carbon nanotubes and N-doped graphene quantum dots-modified (NiMn)Co2O4 使用碳纳米管和掺杂 N 的石墨烯量子点改性 (NiMn)Co2O4 增强超级电容器的电荷存储能力
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-07 DOI: 10.1016/j.jcis.2024.09.039

The integration of ternary metal oxides into carbon materials is anticipated to significantly boost the electrochemical performance of supercapacitor electrodes. This article synthesized carbon nanotubes (CNT)/(NiMn)Co2O4 composite materials using a straightforward hydrothermal method and subsequently prepared composite thin films of CNT/P-(NiMn)Co2O4@NGQD by phosphating and incorporating nitrogen-doped graphene quantum dots (NGQD). These films served as the functional electrode material for supercapacitors, enhancing their performance capabilities. The specific capacity of CNT/P-(NiMn)Co2O4@NGQD was measured at 2172.0 F g−1 at a current density of 1 A g−1, maintaining a capacitance of 1954.0 F g−1 at 10 A g−1, thus demonstrating excellent rate performance. Electrochemical impedance spectroscopy (EIS) further revealed enhancements in electrolyte flow dynamics and capacitance behavior post-NGQD introduction. The energy density of the composite material reached 94.4 Wh kg−1 at power density of 800 W kg−1, demonstrating superior electrochemical performance. The enhancement in these electrochemical properties is attributed to the high specific surface area and active sites of CNT/P-(NiMn)Co2O4@NGQD films, along with the synergistic effects of NGQD and metal ions facilitating rapid electrons and charge transfer. This work provides new insights into developing high-performance supercapacitors.

将三元金属氧化物融入碳材料有望显著提高超级电容器电极的电化学性能。本文采用直接水热法合成了碳纳米管(CNT)/(NiMn)Co2O4 复合材料,随后通过磷化并加入掺氮石墨烯量子点(NGQD)制备了 CNT/P-(NiMn)Co2O4@NGQD 复合薄膜。这些薄膜可用作超级电容器的功能电极材料,从而提高其性能。在电流密度为 1 A g-1 时,CNT/P-(NiMn)Co2O4@NGQD 的比容量为 2172.0 F g-1;在 10 A g-1 时,其电容保持在 1954.0 F g-1,从而表现出优异的速率性能。电化学阻抗谱(EIS)进一步揭示了引入 NGQD 后电解质流动动力学和电容特性的改善。在功率密度为 800 W kg-1 时,复合材料的能量密度达到 94.4 Wh kg-1,显示出卓越的电化学性能。这些电化学性能的提高归功于 CNT/P-(镍锰)Co2O4@NGQD 薄膜的高比表面积和活性位点,以及 NGQD 和金属离子促进快速电子和电荷转移的协同效应。这项工作为开发高性能超级电容器提供了新的思路。
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引用次数: 0
Effect of straw decomposition on hexavalent chromium removal by straw: Significant roles of surface potential and dissolved organic matter 秸秆分解对秸秆去除六价铬的影响:表面电位和溶解有机物的重要作用
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-07 DOI: 10.1016/j.jcis.2024.09.057

Mobility and bioavailability of hexavalent chromium (Cr(VI)) in agricultural soils are affected by interactions between Cr(VI) and returned crop straws. However, the effect of straw decomposition on Cr(VI) removal and underlying mechanisms remain unclear. In this study, Cr(VI) removal by pristine and decomposed rice/rape straws was investigated by batch experiments and a series of spectroscopies. The results showed that straw decomposition inhibited Cr(VI) removal, regardless of straw types. However, the potential mechanisms of the inhibition were distinct for the two straws. For the rice straw, a lower zeta potential after decomposition suppressed Cr(VI) sorption and subsequent reduction. In addition, less Cr(VI) was reduced by the decomposed rice straw-derived dissolved organic matter (DOM) than the pristine one. In contrast, for the rape straw, due to the increased zeta potential after decomposition, the decreased Cr(VI) removal was mainly ascribed to less Cr(VI) reduction by the rape straw-derived DOM. These results emphasized the significant roles of straw surface potential and DOM in Cr(VI) removal, depending on straw types and decomposition, which facilitate the fundamental understanding of Cr(VI) removal by straws and are helpful for predicting the environmental risk of Cr and rational straw return in Cr(VI)-contaminated fields.

农业土壤中六价铬(Cr(VI))的迁移性和生物利用率受到 Cr(VI) 与还田作物秸秆之间相互作用的影响。然而,秸秆分解对六价铬去除的影响及其内在机制仍不清楚。本研究通过间歇实验和一系列光谱分析,研究了原始秸秆和分解后的稻草/秸秆对六价铬的去除作用。结果表明,无论哪种秸秆,秸秆分解都会抑制六价铬的去除。不过,两种秸秆的潜在抑制机制各不相同。对于稻草来说,分解后较低的 zeta 电位抑制了 Cr(VI) 的吸附和随后的还原。此外,与原始稻草相比,分解后的稻草衍生溶解有机物(DOM)对六价铬的还原作用更小。相反,对于油菜秸秆,由于分解后 Zeta 电位增加,六价铬去除率降低主要是由于油菜秸秆衍生的 DOM 对六价铬的还原作用降低。这些结果强调了秸秆表面电位和 DOM 对六价铬去除的重要作用,这取决于秸秆的类型和分解情况,有助于从根本上了解秸秆对六价铬的去除,并有助于预测六价铬的环境风险和在受六价铬污染的田块中合理进行秸秆还田。
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引用次数: 0
Investigation of biodegradable surfactant as a corrosion inhibitor to the cold rolled steel in the membrane separation device process 可生物降解表面活性剂作为膜分离装置工艺中冷轧钢板缓蚀剂的研究
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-07 DOI: 10.1016/j.jcis.2024.09.029

The membrane process is an effective way to realize resource reutilization. Most membrane devices are made of cold-roll steel (CRS), which is easy to corrode when operating in acid conditions. Herein, the biodegradable surfactant dodecyl dimethyl betaine (BS-12) was used as the inhibitor to protect the CRS in the trichloroacetic acid (TCA) solution. The long-term stability membrane tests showed that adding BS-12 will not harm the membrane performance. The weight loss experiments proved that adding BS-12 with trace amount (10 mg·L−1) endowed the CRS with good inhibition efficiency (95.3 %). The electrochemical tests indicated that the mixed inhibitor- BS-12 works by inhibiting the anode and cathode simultaneously, and the polarization resistance increased to 21 times. The SEM, AFM, and CLSM tests proved that adding BS-12 enabled the CRS surface to remain stable. The FTIR and XPS tests proved that BS-12 adsorbed on the CRS surface via physical and chemical adsorption. The theoretical calculations proved the horizontal adsorption of BS-12 on the CRS surface and the existence of the electron transfer within the BS-12 and CRS. The BS-12 showed great potential in the CRS inhibition of the membrane separation and purification processing.

膜工艺是实现资源再利用的有效途径。大多数膜装置由冷轧钢(CRS)制成,在酸性条件下运行时容易腐蚀。本文采用可生物降解的表面活性剂十二烷基二甲基甜菜碱(BS-12)作为抑制剂,以保护三氯乙酸(TCA)溶液中的 CRS。长期稳定性膜测试表明,添加 BS-12 不会损害膜的性能。失重实验证明,添加痕量(10 mg-L-1)的 BS-12 赋予了 CRS 良好的抑制效率(95.3%)。电化学测试表明,混合抑制剂 BS-12 可同时抑制阳极和阴极,极化电阻增加了 21 倍。SEM、AFM 和 CLSM 测试证明,添加 BS-12 可使 CRS 表面保持稳定。傅立叶变换红外光谱和 XPS 测试证明,BS-12 通过物理和化学吸附作用吸附在 CRS 表面。理论计算证明了 BS-12 在 CRS 表面的水平吸附以及 BS-12 和 CRS 内部电子传递的存在。BS-12 在膜分离和纯化处理的 CRS 抑制方面显示出巨大潜力。
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引用次数: 0
Interfacial double-coordination effect reconstructing anode/electrolyte interface for long-term and highly reversible Zn metal anodes 重构阳极/电解质界面的界面双配位效应,实现长期和高度可逆的锌金属阳极
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-07 DOI: 10.1016/j.jcis.2024.09.051

The highly reversible electrochemical deposition and dissolution of zinc metal anode is a critical feature for the practical application of aqueous zinc-ion batteries (ZIBs). Nevertheless, this process is seriously hindered by the uncontrollable electrodeposition and interfacial side reactions caused by thermodynamically unstable anode/electrolyte interface (AEI). Guided by the electrode/electrolyte interface chemistry, thiamine hydrochloride (TH) as a novel additive is added into traditional ZnSO4 (ZS) electrolyte to induce sustained reversible Zn deposition/stripping. Spectroscopic characterizations and electrochemical tests reveal that TH can adsorbed on the anode surface owning to the strong double-coordination effect between N, S atoms and Zn atoms via Zn-N and Zn-S chemical bonds. In addition, there are polar hydroxyl groups in the TH molecular structure which can form hydrogen bonds with water molecules. Thus, the adsorbed TH layer can not only guide the diffusion of Zn2+ ions and achieve dendrite-free electrodeposition process, but also prevent intimate contact between water and anode to suppress the occurrence of interface side reactions. Based on these benefits, the TH additive achieves an ultra-long stable cycle lifespan to 2045 h at 1 mA cm−2 and 1 mAh cm−2. Even at a higher current density of 5 mA cm−2, prolonged cycling performance about 773 h is demonstrated. Besides, the assembled Zn//NVO full cells reveal excellent capacity retention and rate performance under practical conditions, highlighting the efficient and reliable coordination effect of TH additive at the AEI.

锌金属阳极的高度可逆电化学沉积和溶解是水性锌离子电池(ZIB)实际应用的关键特征。然而,热力学上不稳定的阳极/电解质界面(AEI)导致的不可控电沉积和界面副反应严重阻碍了这一过程。在电极/电解质界面化学的指导下,盐酸硫胺(TH)作为一种新型添加剂被添加到传统的 ZnSO4(ZS)电解质中,以诱导持续的可逆锌沉积/剥离。光谱表征和电化学测试表明,由于 N、S 原子与 Zn 原子之间通过 Zn-N 和 Zn-S 化学键存在强烈的双配位效应,TH 可以吸附在阳极表面。此外,TH 分子结构中存在极性羟基,可与水分子形成氢键。因此,吸附的 TH 层不仅能引导 Zn2+ 离子的扩散,实现无枝晶的电沉积过程,还能防止水与阳极的亲密接触,抑制界面副反应的发生。基于这些优点,TH 添加剂在 1 mA cm-2 和 1 mAh cm-2 条件下实现了 2045 小时的超长稳定循环寿命。即使在 5 mA cm-2 的较高电流密度下,也能实现约 773 小时的长期循环性能。此外,组装后的 Zn/NVO 全电池在实际条件下显示出优异的容量保持率和速率性能,凸显了 TH 添加剂在 AEI 上高效可靠的配位效应。
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引用次数: 0
Tandem Pt/TiO2 and Fe3C catalysts for direct transformation of CO2 to light hydrocarbons under high space velocity 串联 Pt/TiO2 和 Fe3C 催化剂用于在高空间速度下将 CO2 直接转化为轻烃
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-07 DOI: 10.1016/j.jcis.2024.09.053

CO2 hydrogenation to hydrocarbons under high space velocity is crucial for industrial applications, but traditional Fe-based catalysts often suffer from the low activity and poor stability. Herein, we report a new tandem catalyst system combining Pt/TiO2 catalysts with Fe3C catalysts for the direct conversion of CO2 into C2-C4 hydrocarbons under high space velocity. The Pt/TiO2 component promotes *CO intermediate production with an enhanced Reverse Water-Gas Shift (RWGS) reaction efficiency, providing a highly reactive species for the Fe3C catalyst to achieve Fischer-Tropsch synthesis (FTS). By maximizing the contact interface between the Pt/TiO2 and Fe-based components through a granule mixing configuration, we achieve significant enhancements in both CO2 conversion rate (24.0 %) and C2-C4 hydrocarbons selectivity (51.1 %) under the gaseous hourly space velocity (GHSV) of 100000 mL gcat−1h−1. Besides, excellent stability is achieved by the tandem catalysts with continuous catalysis for up to 80 h without significant decrease in activity. Through modulation of the reduction states of iron oxide, we effectively tune the composition of Fe-based catalyst, thereby tailoring the product distribution. Through this work, we not only offer a promising avenue for reducing CO2 for efficient CO2 utilization but also highlight the importance of catalyst design in advancing sustainable chemical synthesis.

在高空间速度下将 CO2 加氢转化为碳氢化合物对工业应用至关重要,但传统的铁基催化剂往往存在活性低和稳定性差的问题。在此,我们报告了一种结合了 Pt/TiO2 催化剂和 Fe3C 催化剂的新型串联催化剂体系,用于在高空间速度下将 CO2 直接转化为 C2-C4 碳氢化合物。Pt/TiO2 催化剂能促进 *CO 中间体的生成,提高水气反向变换 (RWGS) 反应的效率,为 Fe3C 催化剂提供高活性物质,从而实现费托合成 (FTS)。通过颗粒混合配置最大限度地提高 Pt/TiO2 和铁基组分之间的接触界面,我们在 100000 mL gcat-1h-1 气体时空速度(GHSV)条件下显著提高了 CO2 转化率(24.0%)和 C2-C4 碳氢化合物选择性(51.1%)。此外,串联催化剂具有极佳的稳定性,可连续催化长达 80 小时而活性不会显著降低。通过调节氧化铁的还原态,我们有效地调节了铁基催化剂的组成,从而调整了产物的分布。通过这项工作,我们不仅为还原二氧化碳以高效利用二氧化碳提供了一条前景广阔的途径,而且突出了催化剂设计在推进可持续化学合成中的重要性。
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引用次数: 0
On-demand green/red light-responsive self-doped SnO2 nanoparticles for single/multi-color transitioning fabrics 用于单色/多色过渡织物的按需绿/红光自掺杂 SnO2 纳米粒子
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-07 DOI: 10.1016/j.jcis.2024.08.226

Semiconductor/redox-based dual light-induced color switching systems (LCSs) with a visible light response at different wavelengths are highly sought after for efficient redox reactions. In this work, Sn2+ self-doped SnO2 has been designed as nanophotocatalysts for preparing visible light-responsive inks/fabrics with single/multi-color abilities. The self-doping of SnO2 nanoparticles results in the formation of oxygen vacancies due to charge compensation effects leading to electron-driven photoreduction and photooxidation of LSC inks. By mixing SnO2-x nanoparticles dispersions with specific redox-sensitive dyes can lead to the creation of well-designed sets of visible light-responsive semiconductor-driven LCS systems with both single-color (RGB) and multi-color (violet and green) changes. The exposure of LCS inks to green (550 nm) light culminates in the rapid photoreduction of the inks to decolorized state, while red (660 nm) light initiates the photooxidation in air. The combination of the LCS inks with –OH-rich polymers can be coated on the hydrophobic surface of the layered fabric to produce photo-responsive fabrics with single/multi-color response. The interaction of green light with the semiconductor-driven LCS systems allows the remote photo-printing of different images/letters on the LCS fabrics. Spontaneous erasure can be achieved by red light with high stability and repeatability (>35 cycles). The research in this paper provides new perspectives and insights for the development of new color-changing materials with potential applications as light-activated sensors and display units.

基于半导体/氧化还原的双光诱导颜色切换系统(LCSs)在不同波长下具有可见光响应,是高效氧化还原反应的理想选择。在这项工作中,设计了 Sn2+ 自掺杂 SnO2 作为纳米光催化剂,用于制备具有单色/多色能力的可见光响应油墨/织物。由于电荷补偿效应,SnO2 纳米粒子的自掺杂会形成氧空位,从而导致 LSC 油墨的电子驱动光还原和光氧化。通过将 SnO2-x 纳米粒子分散体与特定的氧化还原敏感染料混合,可以设计出一套具有单色(RGB)和多色(紫色和绿色)变化的可见光响应型半导体驱动 LCS 系统。将 LCS 油墨置于绿光(550 纳米)下,油墨会迅速光还原至脱色状态,而红光(660 纳米)则会在空气中发生光氧化反应。将 LCS 油墨与富含 -OH 的聚合物结合,涂覆在分层织物的疏水性表面上,可制成具有单色/多色响应的光响应织物。绿光与半导体驱动的 LCS 系统相互作用,可在 LCS 织物上远程光打印不同的图像/字母。红光可实现自发擦除,并具有高稳定性和可重复性(35 个周期)。本文的研究为开发新的变色材料提供了新的视角和见解,这些材料具有作为光激活传感器和显示装置的潜在应用价值。
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引用次数: 0
Ultrathin ternary PtNiRu nanowires for enhanced oxygen reduction and methanol oxidation catalysis via d-band center regulation 通过 d 波段中心调节增强氧还原和甲醇氧化催化的超细三元铂镍钌纳米线
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-07 DOI: 10.1016/j.jcis.2024.09.054

Direct methanol fuel cells rely on the efficiency of their anode/cathode electrocatalysts to facilitate the methanol oxidation reaction and oxygen reduction reaction, respectively. Platinum-based nanocatalysts are at the forefront due to their superior catalytic properties. However, the high-cost, scarcity, and low CO tolerance of platinum pose challenges for the scalable application of DMFCs. Herein, we report novel ultrathin ternary PtNiRu alloy nanowires to improve Pt utilization and CO tolerance. These novel electrocatalysts incorporate the oxophilic metal Ru into ultrathin PtNi nanowires, aiming to enhance the intrinsic activity of platinum while leveraging the long-term durability and high utilization efficiency provided by the bimetallic synergistic effect. The PtNiRu NWs significantly enhance both mass activity and specific activity for ORR, performing about 6.9 times and 3.9 times better than commercial Pt/C, respectively. After a rigorous durability test of 10,000 cycles, the PtNiRu NWs only exhibited a 25.2 % loss in mass activity. Additionally, for MOR, the MA and SA of PtNiRu NWs exceed that of Pt/C catalyst by 4.30 and 2.72 times, respectively, and exhibit exceptional resistance to CO poisoning. Theoretical insights from density functional theory calculations suggest that the introduction of Ru modulates the d-band center of the surface Pt atoms, which contributes to decreased binding strength of oxygenated species and an elevated dissolution potential, substantiating the enhanced performance metrics, and the durability enhancement stems from the stronger PtM bonds than those in PtNiRu NWs resulted from PtRu covalent interactions. These findings not only provide a new perspective on platinum-based nanocatalysts but also significantly advance the quest for more efficient and durable electrocatalysts for DMFCs, representing a substantial stride in fuel cell technology.

直接甲醇燃料电池依靠阳极/阴极电催化剂的效率分别促进甲醇氧化反应和氧气还原反应。铂基纳米催化剂因其卓越的催化特性而处于领先地位。然而,铂的高成本、稀缺性和对 CO 的低耐受性给 DMFC 的规模化应用带来了挑战。在此,我们报告了新型超薄三元铂镍钌合金纳米线,以提高铂的利用率和对一氧化碳的耐受性。这些新型电催化剂在超细铂镍纳米线中加入了亲氧化金属 Ru,旨在提高铂的内在活性,同时利用双金属协同效应提供的长期耐久性和高利用效率。PtNiRu 纳米线显著提高了 ORR 的质量活性和比活性,分别是商用 Pt/C 的 6.9 倍和 3.9 倍。经过 10,000 次的严格耐久性测试后,铂镍钌纳米线的质量活性仅下降了 25.2%。此外,就 MOR 而言,PtNiRu NWs 的 MA 和 SA 分别比 Pt/C 催化剂高出 4.30 倍和 2.72 倍,并表现出卓越的抗 CO 中毒能力。密度泛函理论计算的理论见解表明,Ru 的引入调节了表面铂原子的 d 带中心,从而降低了含氧物种的结合强度并提高了溶解电位,从而证实了性能指标的提高,而耐久性的提高则源于 PtRu 共价相互作用产生的 PtM 键比 PtNiRu NWs 中的 PtM 键更强。这些发现不仅为铂基纳米催化剂提供了新的视角,而且极大地推动了为 DMFCs 寻找更高效、更耐用的电催化剂的工作,标志着燃料电池技术取得了长足进步。
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引用次数: 0
A system for efficient and sustainable cogeneration of water and electricity: Temperature difference induced by photothermal conversion and evaporative cooling 高效、可持续的水电联产系统:光热转换和蒸发冷却引起的温差
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-07 DOI: 10.1016/j.jcis.2024.09.061

Solar energy, with its sustainable properties, has garnered considerable attention for its potential to produce green electricity and clean water. This paper proposes a multistage energy transfer co-generation system (MWCNTs-covered thermoelectric module with aerogel and cooler, AC-CTEM) combining power generation and evaporative cooling. On the light-absorbing surface, the hot side of a thermoelectric module is covered with a hydrophobic coating made of PDMS and MWCNT. The cold side transfers heat to the evaporation zone using a heat sink. Aerogel evaporators are cross-linked with chitosan and polyurethane, which reduces the enthalpy of evaporation and facilitates efficient interfacial evaporation to remove heat and return it to refrigeration. Additionally, with the addition of Fresnel lenses and wind energy to the enhancement device, the system achieved an evaporation rate of 3.445 kg m−2 h−1 and an open-circuit voltage of 201.12 mV under 1 kW m−2 solar irradiation. The AC-CTEM system also demonstrated long-term stability and effectiveness in treating various types of non-potable water. Furthermore, we demonstrated the practical utility of the system by successfully cultivating grass seeds and powering electronic equipment. The AC-CTEM system exemplifies a practical energy-saving approach for the development of highly efficient co-generation systems.

太阳能具有可持续发展的特性,因其生产绿色电力和清洁水的潜力而备受关注。本文提出了一种结合发电和蒸发冷却的多级能量传递联合发电系统(MWCNTs-covered thermoelectric module with aerogel and cooler,AC-CTEM)。在光吸收表面,热电模块的热面覆盖有由 PDMS 和 MWCNT 制成的疏水涂层。冷面利用散热器将热量传递到蒸发区。气凝胶蒸发器与壳聚糖和聚氨酯交联,可降低蒸发焓,促进高效的界面蒸发,从而带走热量并返回制冷。此外,在增强装置中加入菲涅尔透镜和风能后,该系统在 1 kW m-2 太阳辐照下的蒸发率达到 3.445 kg m-2 h-1,开路电压达到 201.12 mV。AC-CTEM 系统在处理各类非饮用水方面也表现出了长期的稳定性和有效性。此外,我们还通过成功培育草籽和为电子设备供电,证明了该系统的实用性。AC-CTEM 系统是开发高效热电联产系统的实用节能方法的典范。
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引用次数: 0
Laser-Generated Au nanoparticles as lithophilic sites in self-supported film host for anode-free lithium metal battery 激光生成的金纳米粒子作为无阳极锂金属电池自支撑膜宿主的亲锂位点
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-07 DOI: 10.1016/j.jcis.2024.09.049

Anode-free lithium metal batteries (AFLMBs) are considered to have greater application potential than traditional LMBs because of their higher energy density and safety. Unfortunately, their poor cycling performances originated from the unsatisfactory reversibility of Li plating/stripping remains a big challenge. A rational designed host for lithium deposition is an effective solving strategy. Herein, pure Au nanoparticles (NPs) without any impurities are prepared by a liquid-phase laser irradiation technology to construct and develop a self-supported Au/reduced graphene oxide (Au/rGO) film as lithium deposition host for AFLMBs. The densely and uniformly distributed Au NPs provide abundant lithiophilic sites that significantly reduce the nucleation barrier of lithium. Attributed to the precise regulation of Au sites towards lithium nucleation/growth, dendrites-free anode and improved electrochemical performance are obtained by using the Au/rGO film host. It keeps stable for 30 min of lithiation at 6 mA cm−2 without dendrite formation. Additionally, the Li||Au/rGO half-cell shows an overpotential close to 0 mV and maintains a Coulombic efficiency exceeding 97 % after 500 cycles at 1 mA cm−2. Moreover, a symmetric Au/rGO-Li cell can operate for 700 h without short-circuit. When paired with LiFePO4 (LFP) to assemble a full battery, the Au/rGO-Li achieves 96 % capacity retention rate after 100 cycles. This work not only develops an efficient host for lithium, but also provides a unique strategy to the safety concerns associated with LMBs’ anodes.

与传统的锂金属电池相比,无阳极锂金属电池(AFLMB)具有更高的能量密度和安全性,因此被认为具有更大的应用潜力。遗憾的是,由于锂镀层/剥离的可逆性不理想,导致其循环性能不佳,这仍然是一个巨大的挑战。合理设计锂沉积宿主是一种有效的解决策略。本文采用液相激光辐照技术制备了不含任何杂质的纯金纳米颗粒(NPs),构建并开发了自支撑金/还原氧化石墨烯(Au/rGO)薄膜作为 AFLMB 的锂沉积宿主。密集均匀分布的金纳米粒子提供了丰富的亲锂位点,大大降低了锂的成核障碍。由于 Au 位点对锂成核/生长的精确调节,使用 Au/rGO 薄膜宿主可获得无树枝状的阳极和更好的电化学性能。它能在 6 mA cm-2 的锂化条件下保持稳定 30 分钟,且不会形成枝晶。此外,Li||Au/rGO 半电池的过电位接近 0 mV,在 1 mA cm-2 下循环 500 次后,库仑效率仍超过 97%。此外,对称的 Au/rGO-Li 电池可以工作 700 小时而不会发生短路。当与磷酸铁锂(LFP)配对组装成完整电池时,Au/rGO-Li 电池在 100 次循环后可达到 96% 的容量保持率。这项工作不仅开发出了一种高效的锂宿主,还为解决与锂聚合物阳极相关的安全问题提供了一种独特的策略。
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引用次数: 0
0D–2D multifunctional bimetallic MOF derivative-MXene heterojunction for high areal capacity lithium-sulfur batteries 0D-2D 多功能双金属 MOF 衍生物-MXene 异质结用于高等容量锂硫电池
IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-09-07 DOI: 10.1016/j.jcis.2024.09.026

Lithium-sulfur (Li-S) batteries have attracted much attention due to their high specific capacity. However, at high loads and rates, the polysulfides conversion rate and ion transport of batteries are slow, limiting their commercialization. This work reports zero-dimensional (0D) bimetallic MOF derivatives grown in situ on two-dimensional (2D) MXene by electrostatic adsorption (FeCo@Ti3C2). The 0D bimetallic structure effectively avoids the stacking of MXene while providing a dual catalytic site for polysulfides. The 2D structure of MXene also provides a large number of pathways for the rapid diffusion of lithium ions. This 0D–2D heterostructured heterogeneous catalyst with bimetallic synergistic active sites efficiently immobilizes and catalyzes polysulfides, providing a fast charge transfer pathway for the electrochemical reaction of lithium polysulfides. The Li-S battery with this multifunctional 0D–2D heterojunction structure catalyst has outstanding high rate capacity (703 mAh g−1 at 4 C at room temperature and 555 mAh g−1 at 2 C at 0 °C), fascinating capacity at high load (5.5 mAh cm−2 after 100 cycles at a high sulfur content of 8.2 mg cm−2). The study provides new ideas for the commercialization of high-efficiency Li-S batteries.

锂硫(Li-S)电池因其高比容量而备受关注。然而,在高负载和高倍率情况下,电池的多硫化物转化率和离子传输速度较慢,限制了其商业化。本研究报告了通过静电吸附在二维(2D)MXene 上原位生长的零维(0D)双金属 MOF 衍生物(FeCo@Ti3C2)。0D 双金属结构有效地避免了 MXene 的堆叠,同时为多硫化物提供了双重催化位点。MXene 的二维结构还为锂离子的快速扩散提供了大量途径。这种 0D-2D 异质结构的异质催化剂具有双金属协同活性位点,可有效固定和催化多硫化物,为多硫化锂的电化学反应提供快速电荷转移途径。采用这种多功能 0D-2D 异质结结构催化剂的锂-S 电池具有出色的高倍率容量(室温下 4 C 时为 703 mAh g-1,0 °C 下 2 C 时为 555 mAh g-1)和高负载时的迷人容量(在 8.2 mg cm-2 的高硫含量条件下循环 100 次后为 5.5 mAh cm-2)。这项研究为高效锂-S 电池的商业化提供了新思路。
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Journal of Colloid and Interface Science
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