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Industrial scaling of molten carbonate electrolytic carbon capture and production of graphene allotropes 熔融碳酸盐电解碳捕获的工业规模化和石墨烯同素异形体的生产
Pub Date : 2025-08-20 DOI: 10.1016/j.decarb.2025.100122
Kyle Hofstetter , Gad Licht , Stuart Licht
The discovery, advances, and industrial-scale up of a unique electrochemical decarbonization chemistry, which sequesters carbon dioxide to mitigate the existential threat of planetary climate change, are presented. C2CNT® (CO2 to Carbon NanoTechnology) is the transition metal nucleated electrolytic splitting of CO2 by its transformation into a wide range of Graphene NanoCarbon allotropes, CGNC, CO2 → ​CGNC ​+ ​O2, such as carbon nanotubes and carbon nano-onions. The original 2015 C2CNT 0.0005 ​m2 electrode process has been scaled to larger than meter-square area electrodes and used in a series of 100 tonne annual CO2 removal industrial Genesis Device modules. The pathway to a further scale-up to a series of 1000 tonne decarbonization placed in series and forming a megaton annual C2CNT decarbonization plant is illustrated.
介绍了一种独特的电化学脱碳化学的发现、进展和工业规模的扩大,这种化学可以隔离二氧化碳,以减轻地球气候变化的生存威胁。C2CNT®(CO2 to Carbon NanoTechnology)是一种过渡金属成核电解分解CO2,将其转化为多种石墨烯纳米碳同素异形体,CGNC, CO2→CGNC + O2,如碳纳米管和碳纳米洋葱。最初的2015 C2CNT 0.0005 m2电极工艺已扩展到大于平方米面积的电极,并用于一系列每年100吨二氧化碳去除工业创世纪设备模块。说明了进一步扩大到一系列1000吨脱碳的途径,这些脱碳系列放置并形成一个百万吨的C2CNT脱碳工厂。
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引用次数: 0
Optimizing lead-free halide perovskites: Strategies for enhanced performance and selectivity in photocatalytic CO2 reduction 优化无铅卤化物钙钛矿:提高光催化CO2还原性能和选择性的策略
Pub Date : 2025-06-02 DOI: 10.1016/j.decarb.2025.100120
Manjing Wang , Daofu Wu , Xiaosheng Tang
Solar energy-powered photocatalytic processes represent a promising avenue for sustainable energy and chemical production. Among these, lead-free halide perovskites (LFHPs) have garnered attention as a next-generation class of photocatalysts for CO2 reduction, offering the advantages of high light absorption and low toxicity. However, the practical application of LFHPs remains constrained by limited catalytic activity and poor product selectivity. This review discusses the advancements in strategies to enhance the catalytic efficiency of LFHPs, such as compositional engineering, surface passivation, and heterostructure formation. These approaches aim to optimize charge carrier dynamics, reduce recombination rates, and improve stability under reaction conditions. Emphasis is also placed on methods to control product selectivity, including tailored reaction environments, co-catalyst integration, and fine-tuning electronic band structures. The discussion extends to key challenges such as material stability under photocatalytic conditions, scalability for industrial applications, and a deeper understanding of reaction mechanisms at the molecular level. Finally, future prospects highlight the critical role of LFHPs in achieving efficient, scalable, and eco-friendly solar-driven chemical synthesis, highlighting their potential to reshape the landscape of sustainable photocatalysis.
太阳能驱动的光催化过程代表了可持续能源和化学生产的一个有前途的途径。其中,无铅卤化物钙钛矿(LFHPs)作为下一代二氧化碳还原光催化剂备受关注,具有高光吸收和低毒性的优点。然而,lfhp的实际应用仍然受到催化活性有限和产物选择性差的限制。本文综述了提高lfhp催化效率的方法,包括组分工程、表面钝化和异质结构的形成。这些方法旨在优化载流子动力学,降低复合速率,提高反应条件下的稳定性。重点还放在控制产品选择性的方法上,包括定制的反应环境,共催化剂集成和微调电子能带结构。讨论扩展到关键挑战,如光催化条件下的材料稳定性,工业应用的可扩展性,以及在分子水平上对反应机制的更深入理解。最后,未来展望强调了lfhp在实现高效、可扩展和环保的太阳能驱动化学合成方面的关键作用,强调了它们重塑可持续光催化景观的潜力。
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引用次数: 0
Synthesis, characterizations, and structure-activity relationship of dual-atom catalysts for CO2 electroreduction CO2电还原双原子催化剂的合成、表征及构效关系
Pub Date : 2025-05-09 DOI: 10.1016/j.decarb.2025.100112
Zhao Li , Xinde Wei , Zhaozhao Zhu , Wu Jiang , Yangwu Hou , Rui Yuan , Yan Wang , Dong Xie , Junjie Wang , Yingxi Lin , Rui Wu , Qingquan Kong , Jun Song Chen
Electrocatalytic carbon dioxide reduction is one of the very effective ways to achieve carbon neutrality, by converting CO2 into fuels and high-value chemicals. Therefore, it is crucial to design efficient CO2 reduction electrocatalysts and understand their reaction mechanism. Among various catalysts, dual-atom catalysts (DACs) offer several advantages, including a wide range of reaction types, high stability, customizable design, high reaction selectivity, tunable electronic structure, and strong catalytic activity. It is thus crucial to understand the reaction mechanism of DACs in CO2 reduction, especially the regulation of critical intermediates. In this review, we focus on the synthesis, structure-activity relationship, and application of DACs. Finally, some challenges and further prospects are also summarized, especially in terms of stability, product selectivity, and large-scale deployment. With the advancement of new materials and computational tools, DACs are poised to play increasingly important roles in CO2 reduction, providing effective solutions for sustainable energy and environmental protection.
通过将二氧化碳转化为燃料和高价值化学品,电催化二氧化碳还原是实现碳中和的非常有效的方法之一。因此,设计高效的CO2还原电催化剂并了解其反应机理至关重要。在各种催化剂中,双原子催化剂具有反应类型广泛、稳定性高、设计可定制、反应选择性高、电子结构可调、催化活性强等优点。因此,了解DACs在CO2还原中的反应机理,特别是对关键中间体的调控是至关重要的。本文就DACs的合成、构效关系及其应用作一综述。最后,总结了该技术在稳定性、产品选择性和大规模部署等方面面临的挑战和未来的发展前景。随着新材料和计算工具的进步,DACs将在二氧化碳减排中发挥越来越重要的作用,为可持续能源和环境保护提供有效的解决方案。
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引用次数: 0
Recent advances of CO2 hydrogenation to methanol 二氧化碳加氢制甲醇的研究进展
Pub Date : 2025-04-29 DOI: 10.1016/j.decarb.2025.100111
Feng Hong , Yanan Qi , Zuodong Yang , Lijun Yu , Xiaoguang Guan , Jiangyong Diao , Bo Sun , Hongyang Liu
The increasingly serious climate issue compels urgent greenhouse gas mitigation strategies. As a budget, plentiful, renewable feedstock and major contributor to global warming, the large-scale catalytic transformation of CO2 has attracted widespread attention from society due to its potential as a solution to the environment and energy crises. At present, catalytic hydrogenation of carbon dioxide to organic chemicals is the primary approach in its industrial applications. In recent decades, various materials containing Cu-, precious metal-, In-, Zn-, and Ga-based catalysts have been designed for CO2 hydrogenation to methanol. Likewise, great advances have been made in CO2-to-chemicals, such as olefins, aromatics, and gasoline by combining CO2-to-CH3OH with methanol transformation or tandem reaction of reverse water-gas shift and Fischer-Tropsch (FT) synthesis. This review exhibits the recent advances in the hydrogenation of CO2-to-CH3OH including the catalyst system, CO2 activation, nature of active sites, intermediate species (formate or carboxyl), structure-activity relationship, and reaction mechanism. Finally, challenges and outlooks in CO2 hydrogenation to methanol are summarized.
日益严重的气候问题迫使我们采取紧急的温室气体减排战略。作为一种廉价、丰富、可再生的原料和全球变暖的主要原因,二氧化碳的大规模催化转化因其解决环境和能源危机的潜力而引起了社会的广泛关注。目前,二氧化碳催化加氢制有机化学品是其工业应用的主要途径。近几十年来,各种含Cu、贵金属、In、Zn和ga基催化剂被设计用于二氧化碳加氢制甲醇。同样,通过将二氧化碳制ch3oh与甲醇转化或逆水气变换串联反应和费托合成相结合,在烯烃、芳烃和汽油等二氧化碳制化学品方面也取得了很大进展。本文综述了近年来CO2加氢制ch3oh的研究进展,包括催化剂体系、CO2活化、活性位点性质、中间产物(甲酸酯或羧基)、构效关系和反应机理。最后,总结了CO2加氢制甲醇的挑战和前景。
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引用次数: 0
The recent progress of high-entropy layered double hydroxides and high-entropy amorphous materials for water electrocatalysis 高熵层状双氢氧化物和高熵非晶态水电催化材料的研究进展
Pub Date : 2025-04-21 DOI: 10.1016/j.decarb.2025.100110
Tadele Hunde Wondimu , Zuo Yong , Akeel A. Shah , Puiki Leung , Yilkal Dessie , Filimon Hadish Abraha , Cristina Flox , Qiang Liao
High-entropy materials (HEMs), which are typically composed of five or more elements in near-equimolar ratios with concentrations ranging from 5 ​% to 35 ​%, have distinct elemental compositions and geometric properties that allow for the development of advanced electrocatalysts for renewable energy conversion systems. The high-entropy effect, crystal dislocations, cocktail effect, and slow diffusion in high-entropy layered double hydroxides (HE-LDHs) and amorphous materials (HE-AMs) have all been shown to boost electrocatalytic water oxidation performance significantly. These materials exhibit remarkable activity and stability in both alkaline and acidic conditions. HE-AMs, in particular, benefit from a variety of defects, including coordinatively unsaturated sites and loosely connected atoms, which are critical to their improved catalytic capabilities. HEMs engineering and precise nanostructure control can address the low intrinsic activity, restricted active sites, and poor conductivity of binary and ternary amorphous and LDH catalysts. This study discusses current advances in HE-LDHs and HE-AMs for water electrolysis, including synthesis methods, structural features, active site identification by DFT calculations, and their applications in water electrocatalysis. The presentation also covers potential problems and future directions for developing these materials in energy conversion device systems.
高熵材料(HEMs)通常由五种或更多元素以接近等摩尔的比例组成,浓度范围为5%至35%,具有独特的元素组成和几何性质,可用于开发用于可再生能源转换系统的高级电催化剂。在高熵层状双氢氧化物(HE-LDHs)和非晶材料(HE-AMs)中,高熵效应、晶体位错、鸡尾酒效应和缓慢扩散都被证明能显著提高电催化水氧化性能。这些材料在碱性和酸性条件下都表现出显著的活性和稳定性。特别是HE-AMs,得益于各种缺陷,包括配位不饱和位点和松散连接的原子,这对它们提高催化能力至关重要。HEMs工程和精确的纳米结构控制可以解决二元和三元非晶和LDH催化剂固有活性低、活性位受限和导电性差的问题。本文讨论了HE-LDHs和HE-AMs在水电解中的研究进展,包括合成方法、结构特点、DFT计算的活性位点鉴定及其在水电催化中的应用。报告还涵盖了在能量转换装置系统中开发这些材料的潜在问题和未来方向。
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引用次数: 0
Progress and future of CO2 conversion based on plasma catalysis 基于等离子体催化的CO2转化研究进展与展望
Pub Date : 2025-04-09 DOI: 10.1016/j.decarb.2025.100109
Lefei Cao, Fei Qi, Nan Zhang, Yayun Pu, Xiaosheng Tang, Qiang Huang
To address the issues of the greenhouse effect and energy dilemma, it is a global hot topic on converting CO2 to valuable chemicals and useable fuels. In this review, firstly, we shortly summarize different CO2 conversion methods including thermal catalysis, biocatalysis, electrocatalysis, photocatalysis, and plasma catalysis. Then, a comprehensive overview of the currently explored plasma driven CO2 conversion is presented, such as microwave discharge plasma, gliding arc discharge plasma, radiofrequency inductively coupled plasma, and dielectric barrier discharge plasma, with an emphasis on their experimental setups, achievements and limitations. Furthermore, the activation of CO2 conversion via the synergistic effect between the plasma and photocatalyst is discussed in detail. Finally, the associated challenges and future development trends for plasma catalytic CO2 conversion are briefly concluded.
为了解决温室效应和能源困境的问题,将二氧化碳转化为有价值的化学品和可用的燃料是一个全球性的热点话题。本文首先综述了不同的CO2转化方法,包括热催化、生物催化、电催化、光催化和等离子体催化。然后,全面概述了目前探索的等离子体驱动CO2转换,如微波放电等离子体、滑动电弧放电等离子体、射频电感耦合等离子体和介质阻挡放电等离子体,重点介绍了它们的实验设置、成就和局限性。此外,还详细讨论了等离子体与光催化剂之间的协同作用对CO2转化的激活作用。最后,简要总结了等离子体催化CO2转化面临的挑战和未来的发展趋势。
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引用次数: 0
Recommended electrochemical measurement protocol for oxygen evolution reaction 建议的氧进化反应电化学测量规程
Pub Date : 2025-04-04 DOI: 10.1016/j.decarb.2025.100108
Chao Wu , Ying Tang , Anqi Zou , Junhua Li , Haoyan Meng , Feng Gao , Jiagang Wu , Xiaopeng Wang
Developing highly active and stable oxygen evolution reaction (OER) catalysts necessitates the establishment of a comprehensive OER catalyst database. However, the absence of a standardized benchmarking protocol has hindered this progress. In this work, we present a systematic protocol for electrochemical measurements to thoroughly evaluate the activity and stability of OER electrocatalysts. We begin with a detailed introduction to constructing the electrochemical system, encompassing experimental setup and the selection criteria for electrodes and electrolytes. Potential contaminants originating from electrolytes, cells, and electrodes are identified and their impacts are discussed. We also examine the effects of external factors, such as temperature, magnetic fields, and natural light, on OER measurements. The protocol outlines operational mechanisms and recommended settings for various electrochemical techniques, including cyclic voltammetry (CV), potentiostatic electrochemical impedance spectroscopy (PEIS), Tafel slope analysis, and pulse voltammetry (PV). We summarize existing evaluation methodologies for assessing intrinsic activities and long-term stabilities of catalysts. Based on these discussions, we propose a comprehensive protocol for evaluating OER electrocatalysts’ performance. Finally, we offer perspectives on advancing OER catalysts from laboratory research to industrial applications.
开发高活性、稳定的析氧反应催化剂需要建立全面的析氧反应催化剂数据库。然而,缺乏标准化的基准测试协议阻碍了这一进展。在这项工作中,我们提出了一个系统的电化学测量方案,以彻底评估OER电催化剂的活性和稳定性。我们首先详细介绍了电化学系统的构建,包括实验设置和电极和电解质的选择标准。潜在的污染物来自电解液,电池和电极的识别和他们的影响进行了讨论。我们还研究了外部因素,如温度、磁场和自然光对OER测量的影响。该协议概述了各种电化学技术的操作机制和推荐设置,包括循环伏安法(CV)、恒电位电化学阻抗谱(PEIS)、塔菲尔斜率分析和脉冲伏安法(PV)。总结了现有的评价催化剂内在活性和长期稳定性的方法。在此基础上,我们提出了一种评价OER电催化剂性能的综合方案。最后,我们提出了推进OER催化剂从实验室研究到工业应用的观点。
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引用次数: 0
Recent advances in interfacial engineering for high-efficiency perovskite photovoltaics 高效钙钛矿光伏电池界面工程研究进展
Pub Date : 2025-03-04 DOI: 10.1016/j.decarb.2025.100107
Zhijie Wang , Cheng Gong , Cong Zhang , Chenxu Zhao , Tzu-Sen Su , Haiyun Li , Hong Zhang
Through strategies such as process optimization, solvent selection, and component tuning, the crystallization of perovskite materials has been effectively controlled, enabling perovskite solar cells (PSCs) to achieve over 25 ​% power conversion efficiency (PCE). However, as PCE continues to improve, interfacial issues within the devices have emerged as critical bottlenecks, hindering further performance enhancements. Recently, interfacial engineering has driven transformative progress, pushing PCEs to nearly 27 ​%. Building upon these developments, this review first summarizes the pivotal role of interfacial modifications in elevating device performance and then, as a starting point, provides a comprehensive overview of recent advancements in normal, inverted, and tandem structure devices. Finally, based on the current progress of PSCs, preliminary perspectives on future directions are presented.
通过工艺优化、溶剂选择和组分调整等策略,有效控制了钙钛矿材料的结晶,使钙钛矿太阳能电池(PSCs)实现了25%以上的功率转换效率(PCE)。然而,随着PCE的不断改进,设备内部的接口问题已经成为阻碍进一步性能增强的关键瓶颈。最近,界面工程推动了变革性的进步,将pce推到了近27%。在这些发展的基础上,本文首先总结了界面修改在提高设备性能方面的关键作用,然后作为起点,全面概述了正常、倒置和串联结构设备的最新进展。最后,根据目前PSCs的研究进展,对其未来发展方向进行了初步展望。
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引用次数: 0
Array structured NiAl-layered double hydroxides grown on graphene by atomic layer deposition as chloride-ion battery cathode 用原子层沉积法在石墨烯上生长阵列结构nial层双氢氧化物作为氯离子电池正极
Pub Date : 2025-02-13 DOI: 10.1016/j.decarb.2025.100106
Guoqing Zhao, Zhen Deng, Gengping Wan, Jinchuan Zhao, Guizhen Wang
Novel and promising chloride ion batteries (CIBs) that can operate at room temperature have attracted great attentions, due to the sustainable chloride-containing resources and high theoretical energy density. To achieve the superior electrochemical properties of CIBs, the structure design of electrode materials is essential. Herein, 2D NiAl-layered double hydroxide (NiAl-LDH) nanoarrays derived from Al2O3 are in-situ grafted to graphene (G) by atomic layer deposition (ALD) and hydrothermal method. The achieved NiAl-LDH@G hybrids with 2D NiAl-LDH arrays grown perpendicularly on graphene surface, can efficiently prevent the stacking of LDHs and enlarge specific surface area to provide more active sites. The NiAl-LDH@G cathode exhibits a maximum discharge capacity of 223.3 ​mA ​h g−1 and an excellent reversible capacity of 107 ​mA ​h g−1 over 500 cycles at 100 ​mA ​g−1 with a high coulombic efficiency around 96 ​%, whereas pure NiAl-LDH has a discharge capacity of only 48.8 ​mA ​h g−1 and a coulombic efficiency (CE) of about 78 ​%. More importantly, the NiAl-LDH@G electrode has a stable voltage at 1.9 ​V and an outstanding discharge capacity of higher than 72 ​mA ​h g−1 after 120 days. Additionally, XRD, XPS, and EDS have been employed to unveil the electrochemical reaction and Cl storage mechanism of the NiAl-LDH@G cathode in CIBs. This work opens a facile and reasonable way for improving electrochemical performance at anion-type rechargeable batteries in terms of cathode material design and mechanism interpretation.
室温下工作的新型氯离子电池因其具有可持续性的含氯资源和较高的理论能量密度而备受关注。为了获得优异的电化学性能,电极材料的结构设计至关重要。本文采用原子层沉积(ALD)和水热法将由Al2O3衍生的二维nial层双氢氧化物(NiAl-LDH)纳米阵列原位接枝到石墨烯(G)上。在石墨烯表面垂直生长的二维NiAl-LDH阵列NiAl-LDH@G杂化体可以有效地防止ldh的堆积,扩大比表面积,提供更多的活性位点。NiAl-LDH@G阴极的最大放电容量为223.3 mA h g−1,在100 mA g−1下循环500次,可逆容量为107 mA h g−1,库仑效率约为96%,而纯NiAl-LDH的放电容量仅为48.8 mA h g−1,库仑效率(CE)约为78%。更重要的是,NiAl-LDH@G电极的电压稳定在1.9 V,放电120天后的放电容量高于72 mA h g−1。此外,利用XRD、XPS和EDS揭示了NiAl-LDH@G阴极在cib中的电化学反应和Cl−储存机理。本研究从正极材料设计和机理解释两方面为提高阴离子型可充电电池的电化学性能开辟了一条简单合理的途径。
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引用次数: 0
Challenges and perspectives toward wide-bandgap perovskite subcell in four-terminal all-perovskite tandem solar cells 四端全钙钛矿串联太阳能电池中宽禁带钙钛矿亚电池的挑战与展望
Pub Date : 2025-01-21 DOI: 10.1016/j.decarb.2025.100098
Hongling Guan , Shiqiang Fu , Weiqing Chen , Weijun Ke , Guojia Fang , Wenlin Feng
Wide-bandgap (WBG) perovskite solar cells (PSCs) have gained remarkable interest owing to their latent applications in tandem solar cells (TSCs). Among them, four-terminal (4T) all-perovskite TSCs have received extensive attention as its do without need to consider current matching, surface roughness, and fabrication processes. However, low open-circuit voltage (VOC) and efficiency of WBG PSCs obstacles their applications in 4T all-perovskite TSCs. Hence, this review firstly discussed the optimizing strategy in perovskite materials layer and properties. Specifically, we assessed the effect of composition, additive and interface engineering on the efficiency and VOC of WBG PSCs. Secondly, the demonstrated applications of different passivation layers designing for intensifying the efficiency of WBG PSCs and 4T all-perovskite TSCs is discussed. Finally, we put forward three specific approaches for future research, in our view, which would offer appropriate guidance for the exploitation of highly efficient and stable 4T all-perovskite TSCs.
宽带隙钙钛矿太阳能电池(PSCs)由于其在串联太阳能电池(TSCs)中的潜在应用而引起了人们的极大兴趣。其中,四端(4T)全钙钛矿tsc由于不需要考虑电流匹配、表面粗糙度和制造工艺而受到广泛关注。然而,低开路电压(VOC)和效率阻碍了WBG psc在4T全钙钛矿tsc中的应用。因此,本文首先讨论了钙钛矿材料层和性能的优化策略。具体而言,我们评估了组成、添加剂和界面工程对WBG聚酰亚酯效率和VOC的影响。其次,讨论了不同钝化层设计在增强WBG PSCs和4T全钙钛矿TSCs效率方面的演示应用。最后,我们提出了未来研究的三种具体方法,我们认为这将为开发高效稳定的4T全钙钛矿tsc提供适当的指导。
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引用次数: 0
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DeCarbon
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