Journal of Energy Chemistry最新文献_第7页

Plasmonic tandem heterojunctions enable high-efficiency charge transfer for broad spectrum photocatalytic hydrogen production 等离子体串联异质结实现了高效电荷转移，可用于广谱光催化制氢

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2024-09-19 DOI: 10.1016/j.jechem.2024.09.018

Rational engineering of semiconductor photocatalysts for efficient hydrogen production is of great significance but still challenging, primarily due to the limitations in charge transfer kinetics. Herein, a fascinating plasmonic tandem heterojunction with the hc-CdS/Mo₂C@C heterostructure is aimfully prepared for effectively promoting the charge separation kinetics of the CdS photocatalyst via the synergistic strategy of phase junction, Schottky junction, and photothermal effect. The difference in atomic configuration between cubic-CdS (c-CdS) and hexagonal-CdS (h-CdS) leads to effective charge separation through a typical II charge transfer mechanism, and plasmonic Schottky junction further extracts the electrons in the hc-CdS phase junction to realize gradient charge transfer. Besides, the photothermal effect of Mo₂C@C helps to expand the light absorption, accelerate charge transfer kinetics, and reduce the hydrogen evolution energy barrier. The carbon layer provides a fast channel for charge transfer and protects the photocatalyst from photocorrosion. As a result, the optimized hc-CMC photocatalyst exhibits a significantly high photocatalytic H₂ production activity of 28.63 mmol/g/h and apparent quantum efficiency of 61.8%, surpassing most of the reported photocatalysts. This study provides a feasible strategy to enhance the charge transfer kinetics and photocatalytic activity of CdS by constructing plasmonic tandem heterogeneous junctions.

半导体光催化剂用于高效制氢的合理工程设计意义重大，但仍具有挑战性，这主要是由于电荷转移动力学的限制。本文旨在通过相结、肖特基结和光热效应的协同策略，制备一种迷人的 hc-CdS/Mo2C@C 异质结构的等离子体串联异质结，以有效促进 CdS 光催化剂的电荷分离动力学。立方CdS（c-CdS）和六方CdS（h-CdS）原子构型的差异通过典型的II电荷转移机制实现了有效的电荷分离，而等离子体肖特基结则进一步提取了hc-CdS相结中的电子，实现了梯度电荷转移。此外，Mo2C@C 的光热效应有助于扩大光吸收，加速电荷转移动力学，降低氢演化能垒。碳层为电荷转移提供了快速通道，并保护光催化剂免受光腐蚀。因此，优化后的 hc-CMC 光催化剂的光催化产氢活性高达 28.63 mmol/g/h，表观量子效率为 61.8%，超过了大多数已报道的光催化剂。这项研究为通过构建等离子体串联异质结来提高 CdS 的电荷转移动力学和光催化活性提供了一种可行的策略。

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引用次数: 0

“One stone, two birds”: Salt template enabling porosity engineering and single metal atom coordinating toward high-performance zinc-ion capacitors "一石二鸟盐模板可实现多孔性工程和单金属原子协调，从而实现高性能锌离子电容器

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2024-09-18 DOI: 10.1016/j.jechem.2024.09.016

Zinc-ion hybrid capacitors (ZIHCs) have received increasing attention as energy storage devices owing to their low cost, high safety, and environmental friendliness. However, their progress has been hampered by low energy and power density, as well as unsatisfactory long-cycle stability, mainly due to the lack of suitable electrode materials. In this context, we have developed manganese single atoms implanted in nitrogen-doped porous carbon nanosheets (MnSAs/NCNs) using a metal salt template method as cathodes for ZIHCs. The metal salt serves a dual purpose in the synthesis process: It facilitates the uniform dispersion of Mn atoms within the carbon matrix and acts as an activating agent to create the porous structure. When applied in ZIHCs, the MnSAs/NCNs electrode demonstrates exceptional performance, including a high capacity of 203 mAh g⁻¹, an energy density of 138 Wh kg⁻¹ at 68 W kg⁻¹, and excellent cycle stability with 91% retention over 10,000 cycles. Theoretical calculations indicate that the introduced Mn atoms modulate the local charge distribution of carbon materials, thereby improving the electrochemical property. This work demonstrates the significant potential of carbon materials with metal atoms in zinc-ion hybrid capacitors, not only in enhancing electrochemical performance but also in providing new insights and methods for developing high-performance energy storage devices.

锌离子混合电容器（ZIHC）因其低成本、高安全性和环境友好性而作为储能设备受到越来越多的关注。然而，由于缺乏合适的电极材料，锌离子混合电容器的发展一直受到能量和功率密度低以及长周期稳定性不理想的阻碍。在此背景下，我们采用金属盐模板法，开发了植入氮掺杂多孔碳纳米片（MnSAs/NCNs）中的锰单原子，作为 ZIHC 的阴极。金属盐在合成过程中具有双重作用：它有助于锰原子在碳基质中的均匀分散，并作为活化剂形成多孔结构。当应用于 ZIHC 时，MnSAs/NCNs 电极表现出了卓越的性能，包括 203 mAh g-1 的高容量、68 W kg-1 时 138 Wh kg-1 的能量密度，以及卓越的循环稳定性（10000 次循环保持率为 91%）。理论计算表明，引入的锰原子调节了碳材料的局部电荷分布，从而改善了电化学性能。这项研究表明，含有金属原子的碳材料在锌离子混合电容器中具有巨大潜力，不仅能提高电化学性能，还能为开发高性能储能器件提供新的见解和方法。

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引用次数: 0

A low redox potential and long life organic anode material for sodium-ion batteries 用于钠离子电池的低氧化还原电位长寿命有机负极材料

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2024-09-17 DOI: 10.1016/j.jechem.2024.09.017

Sodium-ion batteries (SIBs) with organic electrodes are an emerging research direction due to the sustainability of organic materials based on elements like C, H, O, and sodium ions. Currently, organic electrode materials for SIBs are mainly used as cathodes because of their relatively high redox potentials (>1 V). Organic electrodes with low redox potential that can be used as anode are rare. Herein, a novel organic anode material (tetrasodium 1,4,5,8-naphthalenetetracarboxylate, Na₄TDC) has been developed with low redox potential (<0.7 V) and excellent cyclic stability. Its three-sodium storage mechanism was demonstrated with various in-situ/ex-situ spectroscopy and theoretical calculations, showing a high capacity of 208 mAh/g and an average decay rate of merely 0.022% per cycle. Moreover, the Na₄TDC-hard carbon composite can further acquire improved capacity and cycling stability for 1200 cycles even with a high mass loading of up to 20 mg cm⁻². By pairing with a thick Na₃V₂(PO₄)₃ cathode (20.6 mg cm⁻²), the as-fabricated full cell exhibited high operating voltage (2.8 V), excellent rate performance and cycling stability with a high capacity retention of 88.7% after 200 cycles, well highlighting the Na₄TDC anode material for SIBs.

采用有机电极的钠离子电池（SIB）是一个新兴的研究方向，因为基于 C、H、O 和钠离子等元素的有机材料具有可持续性。目前，用于钠离子电池的有机电极材料主要用作阴极，因为它们的氧化还原电位相对较高（1 V）。而氧化还原电位较低且可用作阳极的有机电极却很少见。本文开发了一种新型有机阳极材料（1,4,5,8-萘四甲酸钠，Na4TDC），它具有较低的氧化还原电位（0.7 V）和出色的循环稳定性。通过各种原位/原位光谱和理论计算，证明了它的三钠储存机制，显示出 208 mAh/g 的高容量和每个循环仅 0.022% 的平均衰减率。此外，Na4TDC-硬碳复合材料还能进一步提高容量和循环稳定性，即使质量负载高达 20 mg cm-2，也能维持 1200 个循环。通过与厚Na3V2(PO4)3阴极（20.6 mg cm-2）配对，制备的全电池显示出高工作电压（2.8 V）、优异的速率性能和循环稳定性，200次循环后的容量保持率高达88.7%，充分彰显了Na4TDC阳极材料在SIB中的应用。

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引用次数: 0

Boosting cationic and anionic redox activity of Li-rich layered oxide cathodes via Li/Ni disordered regulation 通过锂/镍无序调节提高富锂层状氧化物阴极的阳离子和阴离子氧化还原活性

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2024-09-17 DOI: 10.1016/j.jechem.2024.09.015

Lithium-rich layered oxides (LLOs) are increasingly recognized as promising cathode materials for next-generation high-energy-density lithium-ion batteries (LIBs). However, they suffer from voltage decay and low initial Coulombic efficiency (ICE) due to severe structural degradation caused by irreversible O release. Herein, we introduce a three-in-one strategy of increasing Ni and Mn content, along with Li/Ni disordering and TM–O covalency regulation to boost cationic and anionic redox activity simultaneously and thus enhance the electrochemical activity of LLOs. The target material, Li_1.2Ni_0.168Mn_0.558Co_0.074O₂ (L1), exhibits an improved ICE of 87.2% and specific capacity of 293.2 mA h g⁻¹ and minimal voltage decay of less than 0.53 mV cycle⁻¹ over 300 cycles at 1C, compared to Li_1.2Ni_0.13Mn_0.54Co_0.13O₂ (Ls) (274.4 mA h g⁻¹ for initial capacity, 73.8% for ICE and voltage decay of 0.84 mV/cycle over 300 cycles at 1C). Theoretical calculations reveal that the density of states (DOS) area near the Fermi energy level for L1 is larger than that of Ls, indicating higher anionic and cationic redox reactivity than Ls. Moreover, L1 exhibits increased O-vacancy formation energy due to higher Li/Ni disordering of 4.76% (quantified by X-ray diffraction Rietveld refinement) and enhanced TM–O covalency, making lattice O release more difficult and thus improving electrochemical stability. The increased Li/Ni disordering also leads to more Ni²⁺ presence in the Li layer, which acts as a pillar during Li⁺ de-embedding, improving structural stability. This research not only presents a viable approach to designing low-Co LLOs with enhanced capacity and ICE but also contributes significantly to the fundamental understanding of structural regulation in high-performance LIB cathodes.

富锂层状氧化物（LLOs）作为下一代高能量密度锂离子电池（LIBs）的正极材料，越来越受到人们的认可。然而，由于不可逆 O 释放导致的严重结构退化，它们存在电压衰减和初始库仑效率（ICE）低的问题。在此，我们引入了一种三合一策略，即增加镍和锰的含量，同时进行锂/镍无序化和 TM-O 共价调节，以同时提高阳离子和阴离子氧化还原活性，从而增强 LLO 的电化学活性。目标材料 Li1.2Ni0.168Mn0.558Co0.074O2 (L1) 的 ICE 提高了 87.2%，比容量达到 293.2 mA h g-1，电压衰减小于 0.相比之下，Li1.2Ni0.13Mn0.54Co0.13O2（Ls）的初始容量为 274.4 mA h g-1，ICE 为 73.8%，在 1C 下循环 300 次的电压衰减为 0.84 mV/周期。理论计算显示，L1 在费米能级附近的状态密度（DOS）区域大于 Ls，这表明其阴离子和阳离子氧化还原反应活性高于 Ls。此外，由于 L1 的锂/镍无序度更高，达到 4.76%（通过 X 射线衍射 Rietveld 精炼量化），且 TM-O 共价性增强，L1 显示出更高的 O 空位形成能，使晶格 O 更难释放，从而提高了电化学稳定性。此外，Li/Ni 无序度的增加还导致 Li 层中存在更多的 Ni2+，在 Li+ 脱嵌过程中起到支柱作用，从而提高了结构的稳定性。这项研究不仅为设计具有更高容量和 ICE 的低 Co LLO 提供了一种可行的方法，而且极大地促进了对高性能 LIB 阴极结构调节的基本理解。

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引用次数: 0

CO2-mediated bicarbonate conversion to concentrated formate in a CEM-based electrolyzer 在基于 CEM 的电解槽中以二氧化碳为媒介将碳酸氢盐转化为浓甲酸盐

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2024-09-17 DOI: 10.1016/j.jechem.2024.09.014

Renewable energy-driven bicarbonate conversion to valuable chemicals presents an attractive strategy for mitigating CO₂ emissions, as bicarbonate can be efficiently generated from the capture of atmospheric CO₂ using alkaline solutions with reactive absorption. In this work, we present a CO₂-mediated bicarbonate conversion to pure formate using a cation exchange membrane-based electrolyzer with a 25 cm² electrode area. Our electrolysis achieved selectivities exceeding 75% for formate at a total current of 2.5 A, achieving formate concentrations up to 1.2 M and yields as high as 95% over extended periods. The techno-economic assessment confirmed the economic viability of the process, highlighting the potential for bicarbonate electrolysis as a sustainable method for producing valuable chemicals.

可再生能源驱动的碳酸氢盐转化为有价值的化学物质为减少二氧化碳排放提供了一种极具吸引力的策略，因为碳酸氢盐可以通过使用具有反应吸收功能的碱性溶液捕获大气中的二氧化碳而高效生成。在这项工作中，我们使用阳离子交换膜电解槽（电极面积为 25 cm2），将二氧化碳介导的碳酸氢盐转化为纯甲酸盐。在总电流为 2.5 A 的情况下，我们的电解法对甲酸盐的选择性超过 75%，甲酸盐浓度高达 1.2 M，长期产量高达 95%。技术经济评估证实了该工艺的经济可行性，突出了碳酸氢盐电解作为生产有价值化学品的可持续方法的潜力。

引用次数: 0

Fabrication of carbon-supported Al2O3 nanoparticles via spontaneous cross-linking to enhance selective hydrogenation of furfural 通过自发交联制备碳支撑 Al2O3 纳米粒子，以提高糠醛的选择性氢化能力

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2024-09-17 DOI: 10.1016/j.jechem.2024.08.059

Selective hydrogenation of furfural to furfuryl alcohol is a great challenge in the hydrogenation field due to thermodynamic preference for hydrogenation of CC over CO. Herein, a novel Al₂O₃/C-u hybrid catalyst, composed of N-modified dendritic carbon networks supporting Al₂O₃ nanoparticles, was successfully prepared via carbonizing the freeze-dried gel from spontaneous cross-linking of alginate, Al³⁺ and urea_. The obtained carbon-supported Al₂O₃ hybrid catalyst has a high ratio (31%) of Al species in pentahedral-coordinated state. The introduction of urea enhances the surface N content, the ratio of pyrrolic N, and specific surface area of catalyst, leading to improved adsorption capacity of CO and the accessibility of active sites. In the furfural hydrogenation reaction with isopropyl alcohol as hydrogen donor, Al₂O₃/C-u catalyst achieved a 90% conversion of furfural with 98.0% selectivity to furfuryl alcohol, outperforming that of commercial γ-Al₂O₃. Moreover, Al₂O₃/C-u demonstrates excellent catalytic stability in the recycling tests attributed to the synergistic effect of abundant weak Lewis acid sites and the anchoring effect of the carbon network on Al₂O₃ nanoparticles. This work provides an innovative and facile strategy for fabrication of carbon-supported Al₂O₃ hybrid catalysts with rich Al^V species, serving as a high selective hydrogenation catalyst through MPV reaction route.

由于热力学上 CC 比 CO 优先加氢，因此将糠醛选择性加氢为糠醇是加氢领域的一大挑战。本文通过对海藻酸盐、Al3+ 和尿素自发交联的冻干凝胶进行碳化，成功制备了一种新型 Al2O3/C-u 混合催化剂，该催化剂由支撑 Al2O3 纳米颗粒的 N 改性树枝状碳网络组成。所获得的碳支撑 Al2O3 混合催化剂中，五面体配位状态的 Al 种类比例较高（31%）。尿素的引入提高了催化剂的表面 N 含量、吡咯烷 N 比例和比表面积，从而提高了 CO 的吸附能力和活性位点的可及性。在以异丙醇为供氢体的糠醛加氢反应中，Al2O3/C-u 催化剂的糠醛转化率达到 90%，对糠醇的选择性达到 98.0%，优于商用 γ-Al2O3 催化剂。此外，Al2O3/C-u 在循环测试中表现出优异的催化稳定性，这归功于丰富的弱路易斯酸位点和碳网络对 Al2O3 纳米颗粒的锚定作用的协同效应。这项工作为制备富含 AlV 物种的碳支撑 Al2O3 混合催化剂提供了一种创新而简便的策略，可通过 MPV 反应路线用作高选择性加氢催化剂。

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引用次数: 0

Optimizing battery deployment: Aging trajectory prediction enabling homogenous performance grouping 优化电池部署：老化轨迹预测实现同质性能分组

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2024-09-16 DOI: 10.1016/j.jechem.2024.09.012

As battery deployments in electric vehicles and energy storage systems grow, ensuring homogeneous performance across units is crucial. We propose a multi-derivative imaging fusion (MDIF) model, employing advanced imaging and machine learning to predict battery aging trajectories from minimal initial data, thus facilitating effective performance grouping before deployment. Utilizing a derivative strategy and Gramian Angular Difference Field for dimensional enhancement, the MDIF model uncovers subtle predictive features from discharge curve data after only ten cycles. The architecture includes a parallel convolutional neural network with lateral connections to enhance feature integration and extraction. Tested on a self-developed dataset, the model achieves an average root-mean-square error of 0.047 Ah and an average mean absolute percentage error of 1.60%, demonstrating high precision and reliability. Its robustness is further validated through transfer learning on two publicly available datasets, adapting with minimal retraining. This approach significantly reduces the testing cycles required, lowering both time and costs associated with battery testing. By enabling precise battery behavior predictions with limited data, the MDIF model optimizes battery utilization and deployment strategies, enhancing system efficiency and sustainability.

随着电动汽车和储能系统中电池部署的增加，确保各单元的性能均匀至关重要。我们提出了一种多衍生成像融合（MDIF）模型，利用先进的成像和机器学习技术，从最少的初始数据中预测电池老化轨迹，从而在部署前进行有效的性能分组。MDIF 模型利用导数策略和格拉米安角差场进行维度增强，仅在十个周期后就能从放电曲线数据中发现微妙的预测特征。该架构包括一个具有横向连接的并行卷积神经网络，以加强特征整合和提取。该模型在自主开发的数据集上进行了测试，其平均均方根误差为 0.047 Ah，平均绝对百分比误差为 1.60%，显示了较高的精度和可靠性。通过在两个公开数据集上进行迁移学习，该模型的稳健性得到了进一步验证，只需最小限度的再训练即可适应。这种方法大大减少了所需的测试周期，降低了与电池测试相关的时间和成本。通过利用有限的数据实现精确的电池行为预测，MDIF 模型优化了电池利用和部署策略，提高了系统效率和可持续性。

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引用次数: 0

A mild, configurable, flexible CoNi-LDH(v)/Zn battery based on H-vacancy-induced reversible Zn2+ intercalation 基于氢空位诱导的可逆 Zn2+ 插层的温和、可配置、灵活的 CoNi-LDH(v)/Zn 电池

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2024-09-16 DOI: 10.1016/j.jechem.2024.09.013

Flexible Zn-based batteries have attracted increasing research interest as essential components of wearable energy storage devices. However, the advancement of flexible aqueous Zn-based batteries based on Co-Ni layered double hydroxide (CoNi-LDH) as the cathode material is hampered by their poor cycling stability and the corrosiveness of alkaline electrolytes. Herein, CoNi-LDH nanosheets enriched with H vacancies (CoNi-LDH_(v)) were constructed on a flexible carbon cloth (CC) substrate via electrochemical deposition and activation. The Zn-based battery comprising CoNi-LDH_(v)@CC as the cathode exhibited highly reversible conversion reactions and stable operation in 3 M ZnSO₄ electrolyte (pH = 4). The battery delivered an excellent specific capacity (225 mA h g⁻¹, 0.26 mA h cm⁻²), acceptable cycling stability (53.9%, 900 cycles), and high discharging voltage. The abundant H vacancies served as active sites for the reversible intercalation of Zn²⁺ and the extravasation of NO₃⁻ generated channels and space for Zn²⁺ transport and storage, together enabling an excellent Zn²⁺ storage capacity. Furthermore, a sandwich-structured solid-state CoNi-LDH_(v)@CC//Zn@CC battery was fabricated and was found to exhibit a noteworthy electrochemical performance and mechanical durability. As a proof of concept, the unencapsulated battery powered a digital watch under various deformation conditions and operated stably for 80 h. Additionally, the flexible battery displayed outstanding customizability, maintaining an open-circuit voltage of 1.42 V even after being cut twice. The proposed engineering strategy contributes to the realization of textiles with truly wearable energy-storage devices.

作为可穿戴储能设备的重要组成部分，柔性锌基电池吸引了越来越多的研究兴趣。然而，以钴镍层状双氢氧化物（CoNi-LDH）为正极材料的柔性锌基水溶液电池循环稳定性差，且易受碱性电解质的腐蚀，这阻碍了其发展。本文通过电化学沉积和活化，在柔性碳布（CC）基底上构建了富含 H 空位（CoNi-LDH(v)）的 CoNi-LDH 纳米片。以 CoNi-LDH(v)@CC 为阴极的锌基电池在 3 M ZnSO4 电解液（pH = 4）中表现出高度可逆的转换反应和稳定的运行。该电池具有出色的比容量（225 mA h g-1，0.26 mA h cm-2）、可接受的循环稳定性（53.9%，900 次循环）和较高的放电电压。丰富的 H 空位是 Zn2+ 可逆插层的活性位点，而 NO3- 的外渗则为 Zn2+ 的传输和储存提供了通道和空间，从而实现了出色的 Zn2+ 储存能力。此外，还制备了一种夹层结构的 CoNi-LDH(v)@CC//Zn@CC 固态电池，并发现该电池具有显著的电化学性能和机械耐久性。作为概念验证，未封装电池在各种变形条件下为数字手表供电，并稳定工作了 80 小时。此外，柔性电池显示出出色的可定制性，即使被切割两次后仍能保持 1.42 V 的开路电压。所提出的工程策略有助于实现具有真正可穿戴储能装置的纺织品。

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引用次数: 0

Few-shot learning for screening 2D Ga2CoS4−x supported single-atom catalysts for hydrogen production 筛选二维 Ga2CoS4-x 支持的单原子制氢催化剂的少量学习方法

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2024-09-16 DOI: 10.1016/j.jechem.2024.09.009

Hydrogen generation and related energy applications heavily rely on the hydrogen evolution reaction (HER), which faces challenges of slow kinetics and high overpotential. Efficient electrocatalysts, particularly single-atom catalysts (SACs) on two-dimensional (2D) materials, are essential. This study presents a few-shot machine learning (ML) assisted high-throughput screening of 2D septuple-atomic-layer Ga₂CoS₄₋_x supported SACs to predict HER catalytic activity. Initially, density functional theory (DFT) calculations showed that 2D Ga₂CoS₄ is inactive for HER. However, defective Ga₂CoS₄₋_x (x = 0–0.25) monolayers exhibit excellent HER activity due to surface sulfur vacancies (SVs), with predicted overpotentials (0–60 mV) comparable to or lower than commercial Pt/C, which typically exhibits an overpotential of around 50 mV in the acidic electrolyte, when the concentration of surface SV is lower than 8.3%. SVs generate spin-polarized states near the Fermi level, making them effective HER sites. We demonstrate ML-accelerated HER overpotential predictions for all transition metal SACs on 2D Ga₂CoS₄₋_x. Using DFT data from 18 SACs, an ML model with high prediction accuracy and reduced computation time was developed. An intrinsic descriptor linking SAC atomic properties to HER overpotential was identified. This study thus provides a framework for screening SACs on 2D materials, enhancing catalyst design.

制氢及相关能源应用在很大程度上依赖于氢进化反应（HER），而氢进化反应面临着动力学速度慢和过电位高的挑战。高效的电催化剂，尤其是二维（2D）材料上的单原子催化剂（SAC）至关重要。本研究通过机器学习（ML）辅助高通量筛选二维七原子层 Ga2CoS4-x 支持的单原子催化剂，预测 HER 催化活性。最初，密度泛函理论（DFT）计算表明，二维 Ga2CoS4 对 HER 没有活性。然而，有缺陷的 Ga2CoS4-x（x = 0-0.25）单层由于表面硫空位（SV）而表现出卓越的 HER 活性，其预测过电位（0-60 mV）与商用 Pt/C 相当或更低，当表面 SV 的浓度低于 8.3% 时，商用 Pt/C 在酸性电解质中通常表现出约 50 mV 的过电位。SV 在费米级附近产生自旋极化态，使其成为有效的 HER 位点。我们展示了二维 Ga2CoS4-x 上所有过渡金属 SAC 的 ML 加速 HER 过电势预测。利用 18 种 SAC 的 DFT 数据，我们开发出了一种预测精度高、计算时间短的 ML 模型。确定了将 SAC 原子特性与 HER 过电势联系起来的内在描述因子。因此，这项研究为筛选二维材料上的 SAC 提供了一个框架，从而提高了催化剂的设计水平。

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引用次数: 0

Green synthesis of glycolic acid through the electrocatalytic reduction of oxalic acid over black TiO2: An experimental and theoretical study 在黑色 TiO2 上通过电催化还原草酸绿色合成乙醇酸：实验和理论研究

IF 13.1 1区化学 Q1 Energy

Journal of Energy Chemistry

Pub Date : 2024-09-16 DOI: 10.1016/j.jechem.2024.09.011

Herein, we present the electrocatalytic four-electron hydrogenation of oxalic acid into glycolic acid using black TiO₂ as an electrocatalyst. Oxalic acid is an abundant compound found in several sources of organic waste. The results showed a high selectivity of black TiO₂ toward glycolic acid, with the formation of glyoxylic acid being the rate-limiting step (glyoxylic acid is the two-electron intermediate). The highest Faradaic efficiency (FE) of 69.6% ± 8.3% was achieved at 10.2 mA cm⁻² in 4 h of electrolysis using an H-type cell operated at room temperature, with 50.2% ± 3.8% of oxalic acid conversion (degradation kinetic constant k = 0.0042 ± 0.0001 min⁻¹), 58.8% ± 7.0% of reaction yield and 1.2 ± 0.18 g L⁻¹ of glycolic acid production. A theoretical model of black TiO₂ coming from anatase TiO₂ was implemented by introducing Ti³⁺ defects, which gave black TiO₂ the theoretical capability to easily transform oxalic acid into glycolic acid as experimentally observed. The reaction mechanism was supported and described in detail by density functional theory calculations, which revealed that surface Ti³⁺ states were the main catalytic sites. This is the first time that a detailed step-by-step mechanism at the atomic level has been proposed for this electrocatalytic reaction, which represents a valuable contribution to the understanding of this process of high energy/environmental interest. This is also the first time that black TiO₂ has been used as an electrocatalyst for this sustainable process.

在此，我们介绍了以黑色 TiO2 为电催化剂将草酸氢化成乙醇酸的电催化四电子氢化过程。草酸是一种存在于多种有机废物中的丰富化合物。研究结果表明，黑色二氧化钛对乙醇酸具有高选择性，乙醛酸的形成是限速步骤（乙醛酸是双电子中间体）。使用室温下运行的 H 型电池，在 10.2 mA cm-2 的条件下电解 4 小时，法拉第效率（FE）最高，为 69.6% ± 8.3%，草酸转化率为 50.2% ± 3.8%（降解动力学常数 k = 0.0042 ± 0.0001 min-1），反应产率为 58.8% ± 7.0%，乙醇酸产量为 1.2 ± 0.18 g L-1。通过引入 Ti3+ 缺陷，实现了由锐钛矿型二氧化钛衍生出黑色二氧化钛的理论模型，从而使黑色二氧化钛理论上能够像实验观察到的那样轻松地将草酸转化为乙醇酸。密度泛函理论计算支持并详细描述了反应机理，发现表面 Ti3+ 状态是主要催化位点。这是首次在原子水平上为这一电催化反应提出详细的分步机理，对理解这一具有高能量/环境意义的过程做出了宝贵贡献。这也是黑色二氧化钛首次被用作这一可持续过程的电催化剂。

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