Carbon Energy最新文献

英文中文

3D‐cavity‐confined CsPbBr3 quantum dots for visible‐light‐driven photocatalytic C(sp3)–H bond activation 用于可见光驱动的光催化 C(sp3)-H 键活化的三维空腔致密 CsPbBr3 量子点

IF 20.5 1区材料科学 Q1 Materials Science

Carbon Energy

Pub Date : 2024-05-15 DOI: 10.1002/cey2.559

Yujie Gao, Handong Jin, D. Esteban, Bo Weng, R. A. Saha, Min-Quan Yang, S. Bals, J. Steele, Haowei Huang, Maarten B. J. Roeffaers

Metal halide perovskite (MHP) quantum dots (QDs) offer immense potential for several areas of photonics research due to their easy and low‐cost fabrication and excellent optoelectronic properties. However, practical applications of MHP QDs are limited by their poor stability and, in particular, their tendency to aggregate. Here, we develop a two‐step double‐solvent strategy to grow and confine CsPbBr3 QDs within the three‐dimensional (3D) cavities of a mesoporous SBA‐16 silica scaffold (CsPbBr3@SBA‐16). Strong confinement and separation of the MHP QDs lead to a relatively uniform size distribution, narrow luminescence, and good ambient stability over 2 months. In addition, the CsPbBr3@SBA‐16 presents a high activity and stability for visible‐light‐driven photocatalytic toluene C(sp3)–H bond activation to produce benzaldehyde with ∼730 µmol g−1 h−1 yield rate and near‐unity selectivity. Similarly, the structural stability of CsPbBr3@SBA‐16 QDs is superior to that of both pure CsPbBr3 QDs and those confined in MCM‐41 with 1D channels.

金属卤化物过氧化物（MHP）量子点（QDs）因其易于制造、成本低廉以及出色的光电特性，为多个光子学研究领域提供了巨大的潜力。然而，MHP QDs 的实际应用却因其稳定性差，特别是容易聚集而受到限制。在此，我们开发了一种分两步进行的双溶剂策略，在介孔 SBA-16 硅支架的三维（3D）空腔（CsPbBr3@SBA-16）中生长和限制 CsPbBr3 QD。MHP QDs 的强封闭性和分离性使其具有相对均匀的尺寸分布、窄发光范围和超过 2 个月的良好环境稳定性。此外，CsPbBr3@SBA-16 在可见光驱动的光催化甲苯 C(sp3)-H键活化生成苯甲醛的过程中具有高活性和稳定性，产率达∼730 µmol g-1 h-1，选择性接近均一。同样，CsPbBr3@SBA-16 QDs 的结构稳定性也优于纯 CsPbBr3 QDs 和封闭在具有 1D 通道的 MCM-41 中的 CsPbBr3 QDs。

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引用次数: 0

Revealing the origin of single‐atom W activity in H2O2 electrocatalytic production: Charge symmetry‐breaking 揭示 H2O2 电催化生产中单原子 W 活性的起源：打破电荷对称性

IF 20.5 1区材料科学 Q1 Materials Science

Carbon Energy

Pub Date : 2024-05-15 DOI: 10.1002/cey2.581

Changfei Jing, Junyang Ding, Peipei Jia, Mengmeng Jin, Lihui Zhou, Xijun Liu, Jun Luo, Sheng Dai

The low‐energy electrochemical production of hydrogen peroxide (H2O2) has garnered significant attention as a viable alternative to traditional industrial routes, with the goal of achieving carbon neutrality. For their H2O2 selectivity in the two‐electron oxygen reduction reaction (ORR), the coordination environment of tungsten (W)‐based materials is critical. In this study, atomically dispersed W single atoms were immobilized on N‐doped carbon substrates by a facile pyrolysis method to obtain a W single‐atom catalyst (W‐SAC). The coordination environment of an isolated W single atom with a tetra‐coordinated porphyrin‐like structure in W‐SAC was determined by X‐ray photoelectron spectroscopy and X‐ray absorption spectroscopy analysis. Notably, the as‐prepared W‐SAC showed superior two‐electron ORR activity in 0.1 M KOH solution, including high onset potential (0.89 V), high H2O2 selectivity (82.5%), and excellent stability. By using differential phase contrast‐scanning transmission electron microscopy and density functional theory calculations, it is revealed that the charge symmetry‐breaking of W atoms changes the adsorption behavior of the intermediates, leading to enhanced reactivity and selectivity for two‐electron ORR. This work broadens the avenue for understanding the charge transfer of W‐based electrocatalytic materials and the in‐depth reaction mechanism of SACs in two‐electron ORR.

过氧化氢（H2O2）的低能耗电化学生产作为传统工业路线的一种可行替代方法，以实现碳中和为目标，引起了广泛关注。在双电子氧还原反应（ORR）中，钨（W）基材料的配位环境对其 H2O2 选择性至关重要。本研究采用简便的热解方法将原子分散的 W 单原子固定在掺杂 N 的碳基底上，从而获得了 W 单原子催化剂（W-SAC）。通过 X 射线光电子能谱和 X 射线吸收光谱分析，确定了 W-SAC 中具有四配位卟啉样结构的孤立 W 单原子的配位环境。值得注意的是，制备的 W-SAC 在 0.1 M KOH 溶液中表现出卓越的双电子 ORR 活性，包括高起始电位（0.89 V）、高 H2O2 选择性（82.5%）和优异的稳定性。通过使用差相对比扫描透射电子显微镜和密度泛函理论计算，发现 W 原子的电荷对称性破坏改变了中间产物的吸附行为，从而提高了双电子 ORR 的反应活性和选择性。这项研究拓宽了人们了解 W 基电催化材料电荷转移的途径，以及 SACs 在双电子 ORR 中的深入反应机理。

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引用次数: 0

In situ high-quality LiF/Li3N inorganic and phenyl-based organic solid electrolyte interphases for advanced lithium–oxygen batteries 用于先进锂-氧电池的原位高质量 LiF/Li3N 无机和苯基有机固态电解质中间体

IF 20.5 1区材料科学 Q1 Materials Science

Carbon Energy

Pub Date : 2024-05-02 DOI: 10.1002/cey2.576

Qianyan Wang, Minsheng Wu, Yunkai Xu, Chuyue Li, Yuanjia Rong, Yaling Liao, Menglin Gao, Xiaoping Zhang, Weirong Chen, Jun Lu

Lithium metal shows a great advantage as the most promising anode for its unparalleled theoretical specific capacity and extremely low electrochemical potential. However, uncontrolled lithium dendrite growth and severe side reactions of the reactive intermediates and organic electrolytes still limit the broad application of lithium metal batteries. Herein, we propose 4-nitrobenzenesulfonyl fluoride (NBSF) as an electrolyte additive for forming a stable organic–inorganic hybrid solid electrolyte interphase (SEI) layer on the lithium surface. The abundance of lithium fluoride and lithium nitride can guarantee the SEI layer's toughness and high ionic conductivity, achieving dendrite-free lithium deposition. Meanwhile, the phenyl group of NBSF significantly contributes to both the chemical stability of the SEI layer and the good adaptation to volume changes of the lithium anode. The lithium–oxygen batteries with NBSF exhibit prolonged cycle lives and excellent cycling stability. This simple approach is hoped to improve the development of the organic–inorganic SEI layer to stabilize the lithium anodes for lithium–oxygen batteries.

金属锂以其无与伦比的理论比容量和极低的电化学电位成为最有前途的负极。然而，锂枝晶的不可控生长以及反应中间体和有机电解质的严重副反应仍然限制了锂金属电池的广泛应用。在此，我们提出用 4-硝基苯磺酰氟（NBSF）作为电解质添加剂，在锂表面形成稳定的有机-无机混合固体电解质相（SEI）层。氟化锂和氮化锂的大量存在保证了 SEI 层的韧性和高离子导电性，实现了无树枝状锂沉积。同时，NBSF 的苯基对 SEI 层的化学稳定性和对锂负极体积变化的良好适应性都有显著贡献。使用 NBSF 的锂-氧电池具有较长的循环寿命和出色的循环稳定性。这种简单的方法有望改善有机-无机 SEI 层的发展，从而稳定锂-氧电池的锂阳极。

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引用次数: 0

Back Cover Image, Volume 6, Number 4, April 2024 封底图片，第 6 卷第 4 号，2024 年 4 月

IF 20.5 1区材料科学 Q1 Materials Science

Carbon Energy

Pub Date : 2024-04-30 DOI: 10.1002/cey2.591

Zhiting Liang, Meng Li, Kai-Hang Ye, Tongxin Tang, Zhan Lin, Yuying Zheng, Yongchao Huang, Hongbing Ji, Shanqing Zhang

Back cover image: BiVO₄ is a promising photoanode material for photoelectrocatalytic water decomposition. However, it still suffers from insufficient photoelectrocatalytic efficiency. Liang et al. introduced Fe-doped carbon nitride to increase the light absorption capacity of BIVO₄ photoanode and double electrode stacking to boost the light utilization rate. This work is beneficial to the design, preparation, and large-scale application of the next generation of high-performance photoanodes.

封底图片：BiVO4 是一种很有前途的光电催化水分解光阳极材料。然而，它仍然存在光电催化效率不足的问题。Liang等人引入了掺杂铁的氮化碳来提高BIVO4光阳极的光吸收能力，并通过双电极堆叠来提高光利用率。这项工作有利于下一代高性能光阳极的设计、制备和大规模应用。

引用次数: 0

Cover Image, Volume 6, Number 4, April 2024 封面图片，第 6 卷第 4 号，2024 年 4 月

IF 20.5 1区材料科学 Q1 Materials Science

Carbon Energy

Pub Date : 2024-04-30 DOI: 10.1002/cey2.590

Meili Guan, Ni Lu, Xuan Zhang, Qiuwan Wang, Jian Bao, Guiye Chen, Hao Yu, Huaming Li, Jiexiang Xia, Xuezhong Gong

Front cover image: Solar-driven CO₂ conversion to solar fuels via semiconductor-photocatalysis is promising, however, it suffers from low selectivity and efficiency due to the lack of desired functionalities of the photocatalyst, and in article number cey2420, Xuezhong Gong et al. demonstrated the selective photoreduction of CO₂ to CO using elaborately fabricated ultrathin Bi₁₂O₁₇Cl₂ nanosheets, identify the functions of bismuth clusters and oxygen vacancies, elucidate synergetic effect, and provide new research approach for preparing smart multi-functional photocatalysts.

封面图片：在cey2420号文章中，Xuezhong Gong等人利用精心制作的超薄Bi12O17Cl2纳米片研究了选择性光催化将CO2转化为CO的过程，确定了铋簇和氧空位的功能。在编号为 cey2420 的文章中，Xuezhong Gong 等人利用精心制作的超薄 Bi12O17Cl2 纳米片证明了 CO2 对 CO 的选择性光还原，确定了铋簇和氧空位的功能，阐明了协同效应，为制备智能多功能光催化剂提供了新的研究方法。

引用次数: 0

Rational design of diamond through microstructure engineering: From synthesis to applications 通过微结构工程合理设计金刚石：从合成到应用

IF 19.5 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon Energy

Pub Date : 2024-04-25 DOI: 10.1002/cey2.570

Yalun Ku, Wentao Huang, Xing Li, Li Wan, Kuikui Zhang, Longbin Yan, Ying Guo, Shaobo Cheng, Chongxin Shan

Diamond possesses excellent thermal conductivity and tunable bandgap. Currently, the high-pressure, high-temperature, and chemical vapor deposition methods are the most promising strategies for the commercial-scale production of synthetic diamond. Although diamond has been extensively employed in jewelry and cutting/grinding tasks, the realization of its high-end applications through microstructure engineering has long been sought. Herein, we discuss the microstructures encountered in diamond and further concentrate on cutting-edge investigations utilizing electron microscopy techniques to illuminate the transition mechanism between graphite and diamond during the synthesis and device constructions. The impacts of distinct microstructures on the electrical applications of diamond, especially the photoelectrical, electrical, and thermal properties, are elaborated. The recently reported elastic and plastic deformations revealed through in situ microscopy techniques are also summarized. Finally, the limitations, perspectives, and corresponding solutions are proposed.

金刚石具有优异的热导率和可调带隙。目前，高压、高温和化学气相沉积法是商业规模生产合成金刚石最有前途的策略。尽管金刚石已被广泛应用于珠宝和切割/研磨工作中，但通过微结构工程实现其高端应用一直是人们追求的目标。在此，我们将讨论金刚石中出现的微观结构，并进一步集中讨论利用电子显微镜技术进行的前沿研究，以阐明石墨和金刚石在合成和器件制造过程中的转变机制。我们详细阐述了不同微观结构对金刚石电气应用的影响，尤其是光电、电气和热性能。此外，还总结了最近报道的通过原位显微镜技术揭示的弹性和塑性变形。最后，提出了局限性、前景和相应的解决方案。

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引用次数: 0

The manipulation of rectifying contact of Co and nitrogen‐doped carbon hierarchical superstructures toward high‐performance oxygen reduction reaction 操纵钴和掺氮碳分层超结构的整流接触实现高性能氧还原反应

IF 20.5 1区材料科学 Q1 Materials Science

Carbon Energy

Pub Date : 2024-04-22 DOI: 10.1002/cey2.529

Jing Li, Tingyu Lu, Yu Fang, Guangyao Zhou, Mingyi Zhang, Huan Pang, Jun Yang, Yawen Tang, Lin Xu

Rational design and construction of oxygen reduction reaction (ORR) electrocatalysts with high activity, good stability, and low price are essential for the practical applications of renewable energy conversion devices, such as metal‐air batteries. Electronic modification through constructing metal/semiconductor Schottky heterointerface represents a powerful strategy to enhance the electrochemical performance. Herein, we demonstrate a concept of Schottky electrocatalyst composed of uniform Co nanoparticles in situ anchored on the carbon nanotubes aligned on the carbon nanosheets (denoted as Co@N‐CNTs/NSs hereafter) toward ORR. Both experimental findings and theoretical simulation testify that the rectifying contact could impel the voluntary electron flow from Co to N‐CNTs/NSs and create an internal electric field, thereby boosting the electron transfer rate and improving the intrinsic activity. As a consequence, the Co@N‐CNTs/NSs deliver outstanding ORR activity, impressive long‐term durability, excellent methanol tolerance, and good performance as the air‐cathode in the Zn‐air batteries. The design concept of Schottky contact may provide the innovational inspirations for the synthesis of advanced catalysts in sustainable energy conversion fields.

合理设计和构建活性高、稳定性好且价格低廉的氧还原反应（ORR）电催化剂对于金属-空气电池等可再生能源转换装置的实际应用至关重要。通过构建金属/半导体肖特基异质界面进行电子改性是提高电化学性能的有力策略。在此，我们展示了一种肖特基电催化剂的概念，它由均匀的钴纳米颗粒原位锚定在排列在碳纳米片上的碳纳米管上（以下简称为 Co@N-CNTs/NSs），以实现 ORR。实验结果和理论模拟都证明，整流接触可以促进电子从 Co 向 N-CNTs/NSs 的自发流动，并产生内部电场，从而提高电子转移率和内在活性。因此，Co@N-CNTs/NSs 具有出色的 ORR 活性、令人印象深刻的长期耐久性、优异的甲醇耐受性，以及在锌-空气电池中作为空气阴极的良好性能。肖特基接触的设计理念可为可持续能源转换领域先进催化剂的合成提供创新灵感。

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引用次数: 0

Enhancing potassium‐ion storage of Bi2S3 through external–internal dual synergism: Ti3C2Tx compositing and Cu2+ doping 通过内外双重协同作用增强 Bi2S3 的钾离子储存：Ti3C2Tx 复合和 Cu2+ 掺杂

IF 20.5 1区材料科学 Q1 Materials Science

Carbon Energy

Pub Date : 2024-04-17 DOI: 10.1002/cey2.563

D. Sha, Yurong You, Rongxiang Hu, Jianxiang Ding, Xin Cao, Yuan Zhang, Long Pan, Zhengming Sun

Potassium‐ion batteries (PIBs) offer a cost‐effective and resource‐abundant solution for large‐scale energy storage. However, the progress of PIBs is impeded by the lack of high‐capacity, long‐life, and fast‐kinetics anode electrode materials. Here, we propose a dual synergic optimization strategy to enhance the K+ storage stability and reaction kinetics of Bi2S3 through two‐dimensional compositing and cation doping. Externally, Bi2S3 nanoparticles are loaded onto the surface of three‐dimensional interconnected Ti3C2Tx nanosheets to stabilize the electrode structure. Internally, Cu2+ doping acts as active sites to accelerate K+ storage kinetics. Various theoretical simulations and ex situ techniques are used to elucidate the external–internal dual synergism. During discharge, Ti3C2Tx and Cu2+ collaboratively facilitate K+ intercalation. Subsequently, Cu2+ doping primarily promotes the fracture of Bi2S3 bonds, facilitating a conversion reaction. Throughout cycling, the Ti3C2Tx composite structure and Cu2+ doping sustain functionality. The resulting Cu2+‐doped Bi2S3 anchored on Ti3C2Tx (C‐BT) shows excellent rate capability (600 mAh g–1 at 0.1 A g–1; 105 mAh g–1 at 5.0 A g–1) and cycling performance (91 mAh g–1 at 5.0 A g–1 after 1000 cycles) in half cells and a high energy density (179 Wh kg–1) in full cells.

钾离子电池（PIB）为大规模能源储存提供了一种成本效益高且资源丰富的解决方案。然而，由于缺乏高容量、长寿命和快速动力学阳极电极材料，钾离子电池的发展受到了阻碍。在此，我们提出了一种双重协同优化策略，通过二维复合和阳离子掺杂来提高 Bi2S3 的 K+ 储存稳定性和反应动力学。从外部看，Bi2S3 纳米颗粒被负载到三维互连的 Ti3C2Tx 纳米片表面，以稳定电极结构。在内部，Cu2+ 的掺杂作为活性位点加速了 K+ 的存储动力学。各种理论模拟和原位技术被用来阐明外部-内部双重协同作用。在放电过程中，Ti3C2Tx 和 Cu2+ 共同促进了 K+ 的插层。随后，Cu2+ 的掺杂主要促进了 Bi2S3 键的断裂，推动了转换反应。在整个循环过程中，Ti3C2Tx 复合结构和 Cu2+ 掺杂保持了功能性。最终在 Ti3C2Tx（C-BT）上锚定的 Cu2+ 掺杂 Bi2S3 在半电池中显示出卓越的速率能力（0.1 A g-1 时为 600 mAh g-1；5.0 A g-1 时为 105 mAh g-1）和循环性能（1000 次循环后 5.0 A g-1 时为 91 mAh g-1），在全电池中显示出较高的能量密度（179 Wh kg-1）。

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引用次数: 0

Deactivation mechanism for water splitting: Recent advances 水分离的失活机制：最新进展

IF 19.5 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Carbon Energy

Pub Date : 2024-04-17 DOI: 10.1002/cey2.528

Yansong Jia, Yang Li, Qiong Zhang, Sohail Yasin, Xinyu Zheng, Kai Ma, Zhengli Hua, Jianfeng Shi, Chaohua Gu, Yuhai Dou, Shixue Dou

Hydrogen (H₂) has been regarded as a promising alternative to fossil-fuel energy. Green H₂ produced via water electrolysis (WE) powered by renewable energy could achieve a zero-carbon footprint. Considerable attention has been focused on developing highly active catalysts to facilitate the reaction kinetics and improve the energy efficiency of WE. However, the stability of the electrocatalysts hampers the commercial viability of WE. Few studies have elucidated the origin of catalyst degradation. In this review, we first discuss the WE mechanism, including anodic oxygen evolution reaction (OER) and cathodic hydrogen evolution reaction (HER). Then, we provide strategies used to enhance the stability of electrocatalysts. After that, the deactivation mechanisms of the typical commercialized HER and OER catalysts, including Pt, Ni, RuO₂, and IrO₂, are summarized. Finally, the influence of fluctuating energy on catalyst degradation is highlighted and in situ characterization methodologies for understanding the dynamic deactivation processes are described.

氢气（H2）一直被视为化石燃料能源的理想替代品。以可再生能源为动力，通过水电解（WE）产生的绿色氢气可实现零碳足迹。人们一直非常关注开发高活性催化剂，以促进水电解反应动力学并提高能源效率。然而，电催化剂的稳定性阻碍了 WE 的商业可行性。很少有研究阐明催化剂降解的原因。在本综述中，我们首先讨论了 WE 的机理，包括阳极氧进化反应 (OER) 和阴极氢进化反应 (HER)。然后，我们提供了用于提高电催化剂稳定性的策略。然后，总结了典型商业化 HER 和 OER 催化剂的失活机理，包括 Pt、Ni、RuO2 和 IrO2。最后，强调了波动能量对催化剂降解的影响，并介绍了了解动态失活过程的原位表征方法。

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引用次数: 0

Biphase‐to‐monophase structure evolution of Na0.766+xLixNi0.33−xMn0.5Fe0.1Ti0.07O2 toward ultradurable Na‐ion batteries 从双相到单相的 Na0.766+xLixNi0.33-xMn0.5Fe0.1Ti0.07O2 结构演化，迈向超耐久镍离子电池

IF 20.5 1区材料科学 Q1 Materials Science

Carbon Energy

Pub Date : 2024-04-17 DOI: 10.1002/cey2.565

Mengting Liu, Zhiwei Cheng, Xu Zhu, Haojie Dong, Tianran Yan, Liang Zhang, Lu Zheng, Hu‐Rong Yao, Xian‐Zuo Wang, Lianzheng Yu, Bing Xiao, Yao Xiao, Peng‐Fei Wang

Layered composite oxide materials with O3/P2 biphasic crystallographic structure typically demonstrate a combination of high capacities of the O3 phase and high operation voltages of the P2 phase. However, their practical applications are seriously obstructed by difficulties in thermodynamic phase regulation, complicated electrochemical phase transition, and unsatisfactory cycling life. Herein, we propose an efficient structural evolution strategy from biphase to monophase of Na0.766+xLixNi0.33−xMn0.5Fe0.1Ti0.07O2 through Li+ substitution. The role of Li+ substitution not only simplifies the unfavorable phase transition by altering the local coordination of transition metal (TM) cations but also stabilizes the cathode–electrolyte interphase to prevent the degradation of TM cations during battery cycling. As a result, the thermodynamically robust O3‐Na0.826Li0.06Ni0.27Mn0.5Fe0.1Ti0.07O2 cathode delivers a high capacity of 139.4 mAh g−1 at 0.1 C and shows prolonged cycling life at high rates, with capacity retention of 81.6% at 5 C over 500 cycles. This work establishes a solid relationship between the thermodynamic structure evolution and electrochemistry of layered cathode materials, contributing to the development of long‐life sodium‐ion batteries.

具有 O3/P2 双相晶体结构的层状复合氧化物材料通常兼具 O3 相的高容量和 P2 相的高工作电压。然而，由于热力学相调节困难、电化学相变复杂、循环寿命不理想等原因，这些材料的实际应用受到严重阻碍。在此，我们提出了一种通过 Li+ 替代实现 Na0.766+xLixNi0.33-xMn0.5Fe0.1Ti0.07O2 从双相到单相的高效结构演化策略。Li+ 取代的作用不仅是通过改变过渡金属阳离子的局部配位来简化不利相变，而且还能稳定阴极-电解质间相，防止过渡金属阳离子在电池循环过程中降解。因此，热力学上稳健的 O3-Na0.826Li0.06Ni0.27Mn0.5Fe0.1Ti0.07O2 阴极在 0.1 摄氏度时可提供 139.4 mAh g-1 的高容量，并在高速率下显示出更长的循环寿命，在 5 摄氏度下循环 500 次后容量保持率为 81.6%。这项研究在层状阴极材料的热力学结构演化和电化学之间建立了牢固的关系，有助于长寿命钠离子电池的开发。

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