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Sulfur and carbon co-doped g-C3N4 microtubes with enhanced photocatalytic H2 production activity 硫碳共掺杂g-C3N4微管增强光催化制氢活性
IF 3.1 4区 工程技术 Q3 ENERGY & FUELS Pub Date : 2023-10-20 DOI: 10.1007/s11708-023-0899-z
Yang Ge, Quanhao Shen, Qi Zhang, Naixu Li, Danchen Lu, Zhaoming Zhang, Zhiwei Fu, Jiancheng Zhou

Metal-free graphitic carbon nitride (g-C3N4) has captured significant attention as a low-cost and efficient hydrogen production photocatalyst through. Effectively regulating the microstructure and accelerating the separation of photogenerated carriers remain crucial strategies for promoting the photocatalytic performance of this material. Herein, a novel sulfur–carbon co-doped g-C3N4 (SCCN) hierarchical microtubules filled with abundant nanosheets inside by thermal polymerization is reported. Numerous nanosheets create abundant pores and cavities inside the SCCN microtubes, thereby increasing the specific surface area of g-C3N4 and providing sufficient reactant attachment sites. Besides, the hierarchical structure of SCCN microtubules strengthens the reflection and scattering of light, and the utilization of visible light is favorably affected. More importantly, co-doping S and C has greatly improved the photocatalytic performance of graphitic carbon nitride, optimized the band gap structure and enhanced the photogenerated carrier splitting. Consequently, the SCCN exhibits a remarkable photocatalytic H2 evolution rate of 4868 µmol/(g·h). This work demonstrates the potential of multi-nonmetal doped g-C3N4 as the ideal photocatalyst for H2 evolution.

无金属石墨氮化碳(g-C3N4)作为一种低成本、高效的光催化剂已经引起了人们的广泛关注。有效调控光生载体的微观结构和加速其分离是提高该材料光催化性能的关键策略。本文报道了一种新型的硫碳共掺杂g-C3N4 (SCCN)微管,其内部填充了丰富的纳米片。大量的纳米片在SCCN微管内部形成了丰富的孔和空腔,从而增加了g-C3N4的比表面积,并提供了足够的反应物附着位点。此外,SCCN微管的层次化结构增强了光的反射和散射,有利于可见光的利用。更重要的是,共掺杂S和C大大提高了石墨氮化碳的光催化性能,优化了带隙结构,增强了光生载流子的分裂。结果表明,SCCN的光催化析氢速率为4868µmol/(g·h)。这一工作证明了多种非金属掺杂g-C3N4作为理想的析氢光催化剂的潜力。
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引用次数: 0
Automotive revolution and carbon neutrality 汽车革命与碳中和
IF 3.1 4区 工程技术 Q3 ENERGY & FUELS Pub Date : 2023-10-20 DOI: 10.1007/s11708-023-0890-8
C. C. Chan, Wei Han, Hanlei Tian, Yanbing Liu, Tianlu Ma, C. Q. Jiang

The automotive industry is in the midst of a groundbreaking revolution, driven by the imperative to achieve intelligent driving and carbon neutrality. A crucial aspect of this transformation is the transition to electric vehicles (EVs), which necessitates widespread changes throughout the entire automotive ecosystem. This paper examines the challenges and opportunities of this transition, including automotive electrification, intelligence-connected transportation system, and the potential for new technologies such as hydrogen fuel cells. Meanwhile, it discusses the key technologies and progress of the hydrogen energy industry chain in the upstream hydrogen production, midstream hydrogen storage and transportation, downstream hydrogen station construction and hydrogen fuel cells in turn. Finally, it proposes the directions for future layout, providing guidance for future development.

在实现智能驾驶和碳中和的当务之急的推动下,汽车行业正处于一场划时代的革命之中。这场变革的一个重要方面是向电动汽车(EV)的过渡,这就需要对整个汽车生态系统进行广泛变革。本文探讨了这一转型的挑战和机遇,包括汽车电气化、智能互联交通系统以及氢燃料电池等新技术的潜力。同时,本文从上游制氢、中游储运、下游加氢站建设和氢燃料电池四个方面,依次探讨了氢能产业链的关键技术和进展。最后,提出了未来的布局方向,为未来发展提供指导。
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引用次数: 0
Electrochemical CO2 reduction to C2+ products over Cu/Zn intermetallic catalysts synthesized by electrodeposition 在电沉积法合成的铜/锌金属间催化剂上电化学还原二氧化碳至 C2+ 产物
IF 3.1 4区 工程技术 Q3 ENERGY & FUELS Pub Date : 2023-10-20 DOI: 10.1007/s11708-023-0898-0
Ting Deng, Shuaiqiang Jia, Shitao Han, Jianxin Zhai, Jiapeng Jiao, Xiao Chen, Cheng Xue, Xueqing Xing, Wei Xia, Haihong Wu, Mingyuan He, Buxing Han

Electrocatalytic CO2 reduction (ECR) offers an attractive approach to realizing carbon neutrality and producing valuable chemicals and fuels using CO2 as the feedstock. However, the lack of cost-effective electrocatalysts with better performances has seriously hindered its application. Herein, a one-step co-electrodeposition method was used to introduce Zn, a metal with weak *CO binding energy, into Cu to form Cu/Zn intermetallic catalysts (Cu/Zn IMCs). It was shown that, using an H-cell, the high Faradaic efficiency of C2+ hydrocarbons/alcohols (({rm{F}}{{rm{E}}_{{{rm{C}}_{2 + }}}})) could be achieved in ECR by adjusting the surface metal components and the applied potential. In suitable conditions, FEC2+ and current density could be as high as 75% and 40 mA/cm2, respectively. Compared with the Cu catalyst, the Cu/Zn IMCs have a lower interfacial charge transfer resistance and a larger electrochemically active surface area (ECSA), which accelerate the reaction. Moreover, the *CO formed on Zn sites can move to Cu sites due to its weak binding with *CO, and thus enhance the C–C coupling on the Cu surface to form C2+ products.

电催化二氧化碳还原(ECR)为实现碳中和以及以二氧化碳为原料生产有价值的化学品和燃料提供了一种极具吸引力的方法。然而,由于缺乏性价比高、性能更好的电催化剂,严重阻碍了其应用。本文采用一步共电泳法,在铜中引入具有弱*CO结合能的金属 Zn,形成 Cu/Zn 金属间催化剂(Cu/Zn IMCs)。研究表明,在 ECR 中使用 H 细胞,通过调整表面金属成分和外加电势,可以实现 C2+ 碳氢化合物/酒精的高法拉第效率(({rm{F}}{{rm{E}}_{{rm{C}}_{2 + }}}}))。在合适的条件下,FEC2+ 和电流密度可分别高达 75% 和 40 mA/cm2。与铜催化剂相比,铜/锌 IMC 具有更低的界面电荷转移电阻和更大的电化学活性表面积(ECSA),从而加速了反应。此外,由于 Zn 与 *CO 的结合力较弱,在 Zn 位点上形成的 *CO 可以移动到 Cu 位点,从而增强 Cu 表面的 C-C 偶联,形成 C2+ 产物。
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引用次数: 0
Emerging trends in self-healable nanomaterials for triboelectric nanogenerators: A comprehensive review and roadmap 用于三电纳米发电机的自修复纳米材料的新趋势:全面回顾与路线图
IF 3.1 4区 工程技术 Q3 ENERGY & FUELS Pub Date : 2023-09-30 DOI: 10.1007/s11708-023-0896-2
Prabhakar Yadav, Kuldeep Sahay, Malvika Srivastava, Arpit Verma, Bal Chandra Yadav

A thorough analysis of triboelectric nanogenerators (TENGs) that make use of self-healable nanomaterials is presented in this review. These TENGs have shown promise as independent energy sources that do not require an external power source to function. TENGs are developing into a viable choice for powering numerous applications as low-power electronics technology advances. Despite having less power than conventional energy sources, TENGs do not directly compete with these. TENGs, on the other hand, provide unique opportunities for future self-powered systems and might encourage advancements in energy and sensor technologies. Examining the many approaches used to improve nanogenerators by employing materials with shape memory and self-healable characteristics is the main goal of this review. The findings of this comprehensive review provide valuable information on the advancements and possibilities of TENGs, which opens the way for further research and advancement in this field. The discussion of life cycle evaluations of TENGs provides details on how well they perform in terms of the environment and identifies potential improvement areas. Additionally, the cost-effectiveness, social acceptability, and regulatory implications of self-healing TENGs are examined, as well as their economic and societal ramifications.

本综述全面分析了利用可自修复纳米材料的三电纳米发电机(TENGs)。这些 TENG 已显示出作为独立能源的前景,无需外部电源即可发挥作用。随着低功耗电子技术的发展,TENGs 正在成为众多应用的可行供电选择。尽管 TENG 的功率低于传统能源,但并不直接与传统能源竞争。另一方面,TENG 为未来的自供电系统提供了独特的机会,并可能促进能源和传感器技术的进步。本综述的主要目的是研究通过采用具有形状记忆和自修复特性的材料来改进纳米发电机的多种方法。本综述的结论为 TENGs 的进步和可能性提供了宝贵的信息,为该领域的进一步研究和进步开辟了道路。对 TENGs 生命周期评估的讨论详细说明了 TENGs 在环境方面的表现,并确定了潜在的改进领域。此外,还研究了自愈式腾博会登录的成本效益、社会可接受性和监管影响,以及其经济和社会影响。
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引用次数: 0
Conversion of polyethylene to gasoline: Influence of porosity and acidity of zeolites 聚乙烯转化为汽油:沸石孔隙率和酸度的影响
IF 3.1 4区 工程技术 Q3 ENERGY & FUELS Pub Date : 2023-09-30 DOI: 10.1007/s11708-023-0897-1
Chunyu Li, Haihong Wu, Ziyu Cen, Wanying Han, Xinrui Zheng, Jianxin Zhai, Jiao Xu, Longfei Lin, Mingyuan He, Buxing Han

Plastic waste is causing serious environmental problems. Developing efficient, cheap and stable catalytic routes to convert plastic waste into valuable products is of great importance for sustainable development, but remains to be a challenging task. Zeolites are cheap and stable, but they are usually not efficient for plastic conversion at a low temperature. Herein a series of microporous and mesoporous zeolites were used to study the influence of porosity and acidity of zeolite on catalytic activity for plastics conversion. It was observed that H-Beta zeolite was an efficient catalyst for cracking high-density polyethylene to gasoline at 240 °C, and the products were almost C4-C12 alkanes. The effect of porosity and acidity on catalytic performance of zeolites was evaluated, which clearly visualized the good performance of H-Beta due to high surface area, large channel system, large amount accessible acidic sites. This study provides very useful information for designing zeolites for efficient conversion of plastics.

塑料垃圾正在引发严重的环境问题。开发高效、廉价和稳定的催化途径,将塑料废弃物转化为有价值的产品,对可持续发展具有重要意义,但仍是一项具有挑战性的任务。沸石既便宜又稳定,但在低温条件下通常不能有效地进行塑料转化。本文使用一系列微孔和介孔沸石来研究沸石的孔隙率和酸度对塑料转化催化活性的影响。结果表明,H-Beta 沸石是一种高效催化剂,可在 240 ℃ 下将高密度聚乙烯裂解为汽油,产物几乎为 C4-C12 烷烃。研究还评估了孔隙率和酸度对沸石催化性能的影响,结果表明 H-Beta 沸石具有高比表面、大通道系统和大量可访问的酸性位点,因而具有良好的催化性能。这项研究为设计高效转化塑料的沸石提供了非常有用的信息。
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引用次数: 0
Formic acid dehydrogenation reaction on high-performance PdxAu1−x alloy nanoparticles prepared by the eco-friendly slow synthesis methodology 环保型慢合成法制备的高性能 PdxAu1-x 合金纳米粒子上的甲酸脱氢反应
IF 3.1 4区 工程技术 Q3 ENERGY & FUELS Pub Date : 2023-09-16 DOI: 10.1007/s11708-023-0895-3
Yibo Gao, Erjiang Hu, Bo Huang, Zuohua Huang

Dehydrogenation of formic acid (FA) is considered to be an effective solution for efficient storage and transport of hydrogen. For decades, highly effective catalysts for this purpose have been widely investigated, but numerous challenges remain. Herein, the PdxAu1−x (x = 0, 0.2, 0.4, 0.5, 0.6, 0.8, 1) alloys over the whole composition range were successfully prepared and used to catalyze FA hydrogen production efficiently near room temperature. Small PdAu nanoparticles (5–10 nm) were well-dispersed and supported on the activated carbon to form PdAu solid solution alloys via the eco-friendly slow synthesis methodology. The physicochemical properties of the PdAu alloys were comprehensively studied by utilizing various measurement methods, such as X-ray diffraction (XRD), N2 adsorption–desorption, high angle annular dark field-scanning transmission electron microscope (HAADF-STEM), X-ray photoelectrons spectroscopy (XPS). Notably, owing to the strong metal-support interaction (SMSI) and electron transfer between active metal Au and Pd, the Pd0.5Au0.5 obtained exhibits a turnover frequency (TOF) value of up to 1648 h−1 (313 K, nPd+Au/nFA = 0.01, nHCOOH/nHCOONa = 1:3) with a high activity, selectivity, and reusability in the FA dehydrogenation.

甲酸(FA)脱氢被认为是高效储存和运输氢气的有效解决方案。数十年来,人们一直在广泛研究用于这一目的的高效催化剂,但仍面临诸多挑战。在此,我们成功制备了整个成分范围内的 PdxAu1-x(x = 0、0.2、0.4、0.5、0.6、0.8、1)合金,并将其用于在室温附近高效催化 FA 制氢。通过生态友好的缓慢合成方法,小的 PdAu 纳米颗粒(5-10 nm)被很好地分散并支撑在活性炭上形成 PdAu 固溶体合金。利用 X 射线衍射 (XRD)、N2 吸附-解吸、高角度环形暗场扫描透射电子显微镜 (HAADF-STEM)、X 射线光电子能谱 (XPS) 等多种测量方法对 PdAu 合金的理化性质进行了全面研究。值得注意的是,由于活性金属 Au 和 Pd 之间强烈的金属-支撑相互作用(SMSI)和电子传递,获得的 Pd0.5Au0.5 在 FA 脱氢过程中显示出高达 1648 h-1 的周转频率(TOF)值(313 K,nPd+Au/nFA = 0.01,nHCOOH/nHCOONa = 1:3),具有高活性、高选择性和可重复使用性。
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引用次数: 0
Function-reversible facets enabling SrTiO3 nanocrystals for improved photocatalytic hydrogen evolution 功能可逆面使 SrTiO3 纳米晶体能够改善光催化氢气进化性能
IF 3.1 4区 工程技术 Q3 ENERGY & FUELS Pub Date : 2023-09-10 DOI: 10.1007/s11708-023-0894-4
Bin Wang, Bei An, Xiaoqian Li, Shaohua Shen

It has been widely reported that, for faceted nanocrystals, the two adjacent facets with different band levels contribute to promoted charge separation, and provide active sites for photocatalytic reduction and oxidation reaction, respectively. In such cases, only one family of facets can be used for photocatalytic hydrogen evolution. Herein, by using SrTiO3 nanocrystals enclosed by {023} and {001} facets as a model photocatalyst, this paper proposed a strategy to achieve the full-facets-utilization of the nanocrystals for photocatalytic hydrogen via chemically depositing Pt nanoparticles on all facets. The photo-deposition experiment of CdS provided direct evidence to demonstrate that the {023} facets which were responsible for photooxidation reaction can be function-reversed for photocatalytic hydrogen evolution after depositing Pt nanoparticles, together with the {001} facets. Thus, the full-facets-utilization led to a much-improved activity for photocatalytic hydrogen, in contrast to those SrTiO3 nanocrystals with only {001} facets deposited by Pt nanoparticles via a photo-deposition method.

据广泛报道,对于刻面纳米晶体而言,具有不同能带水平的相邻两个刻面有助于促进电荷分离,并分别为光催化还原和氧化反应提供活性位点。在这种情况下,只有一种刻面可用于光催化氢进化。本文以钛酸锶(SrTiO3)纳米晶体的{023}和{001}面为光催化剂模型,提出了一种在纳米晶体的所有面上化学沉积铂纳米颗粒的策略,以实现纳米晶体全面利用光催化氢。CdS 的光沉积实验提供了直接证据,证明了在沉积铂纳米颗粒后,负责光氧化反应的 {023} 面和 {001} 面可以实现功能逆转,用于光催化氢气进化。因此,与铂纳米粒子通过光沉积法沉积的仅有{001}面的钛酸锶纳米晶体相比,利用全刻面可大大提高光催化氢气的活性。
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引用次数: 0
Surface modification by ligand growth strategy for dense copper bismuth film as photocathode to enhance hydrogen production activity 通过配体生长策略对作为光电阴极的致密铜铋薄膜进行表面改性以提高制氢活性
IF 3.1 4区 工程技术 Q3 ENERGY & FUELS Pub Date : 2023-08-30 DOI: 10.1007/s11708-023-0893-5
Zhouzhou Wang, Qingwei Wu, Jieming Wang, Ying Yu

Hydrogen production from photoelectrochemical (PEC) water splitting has been regarded as a promising way to utilize renewable and endless solar energy. However, semiconductor film grown on photoelectrode suffers from numerous challenges, leading to the poor PEC performance. Herein, a straightforward sol-gel method with the ligand-induced growth strategy was employed to obtain dense and homogeneous copper bismuthate photocathodes for PEC hydrogen evolution reaction. By various characterizations, it was found that the nucleation and surface growth of CuBi2O4 layer induced by 2-methoxyethanol ligand (2-CuBi2O4) demonstrated a decent crystallinity and coverage, as well as a large grain size and a low oxygen vacancy concentration, leading to the good ability of light absorption and carrier migration. Consequently, under simulated sunlight irradiation (AM1.5G, 100 mW/cm2), the 2-CuBi2O4 photocathode achieved an enhanced photocurrent density of −1.34 mA·cm−2 at 0.4 V versus the reversible hydrogen electrode and a promising applied bias photon-to-current efficiency of 0.586%. This surface modification by ligand growth strategy will shed light on the future design of advanced photoelectrodes for PEC water splitting.

光电化学(PEC)水分裂制氢被认为是利用可再生和无穷无尽的太阳能的一种有前途的方法。然而,在光电电极上生长的半导体薄膜面临诸多挑战,导致 PEC 性能不佳。本文采用配体诱导生长策略的直接溶胶-凝胶法,获得了用于 PEC 氢气进化反应的致密均匀的铜铋酸盐光电阴极。通过各种表征发现,在 2-甲氧基乙醇配体(2-CuBi2O4)的诱导下,CuBi2O4 层的成核和表面生长表现出良好的结晶度和覆盖率,以及较大的晶粒尺寸和较低的氧空位浓度,从而具有良好的光吸收和载流子迁移能力。因此,在模拟太阳光照射(AM1.5G,100 mW/cm2)下,2-CuBi2O4 光阴极在 0.4 V 时的光电流密度比可逆氢电极高出 -1.34 mA-cm-2,应用偏压光子对电流效率达到 0.586%。这种通过配体生长进行表面改性的策略将为未来设计用于 PEC 水分离的先进光电极提供启示。
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引用次数: 0
Production of hydrogen from fossil fuel: A review 化石燃料制氢研究进展
IF 2.9 4区 工程技术 Q3 ENERGY & FUELS Pub Date : 2023-08-20 DOI: 10.1007/s11708-023-0886-4
Shams Anwar, Xianguo Li

Production of hydrogen, one of the most promising alternative clean fuels, through catalytic conversion from fossil fuel is the most technically and economically feasible technology. Catalytic conversion of natural gas into hydrogen and carbon is thermodynamically favorable under atmospheric conditions. However, using noble metals as a catalyst is costly for hydrogen production, thus mandating non-noble metal-based catalysts such as Ni, Co, and Cu-based alloys. This paper reviews the various hydrogen production methods from fossil fuels through pyrolysis, partial oxidation, autothermal, and steam reforming, emphasizing the catalytic production of hydrogen via steam reforming of methane. The multicomponent catalysts composed of several nonnoble materials have been summarized. Of the Ni, Co, and Cu-based catalysts investigated in the literature, Ni/Al2O3 catalyst is the most economical and performs best because it suppresses the coke formation on the catalyst. To avoid carbon emission, this method of hydrogen production from methane should be integrated with carbon capture, utilization, and storage (CCUS). Carbon capture can be accomplished by absorption, adsorption, and membrane separation processes. The remaining challenges, prospects, and future research and development directions are described.

氢是最有前途的替代清洁燃料之一,通过化石燃料的催化转化生产氢是技术上和经济上最可行的技术。在大气条件下,天然气催化转化为氢和碳在热力学上是有利的。然而,使用贵金属作为催化剂生产氢气的成本很高,因此要求使用非贵金属基催化剂,如Ni, Co和cu基合金。综述了化石燃料制氢的各种方法,包括热解、部分氧化、自热和蒸汽重整,重点介绍了甲烷蒸汽重整催化制氢的方法。综述了几种非贵金属材料组成的多组分催化剂。在文献中研究的Ni, Co和cu基催化剂中,Ni/Al2O3催化剂是最经济且性能最好的,因为它抑制了催化剂上的焦炭形成。为了避免碳排放,这种甲烷制氢的方法应该与碳捕获、利用和储存(CCUS)相结合。碳捕获可以通过吸收、吸附和膜分离过程来完成。展望了当前面临的挑战和未来的研究与发展方向。
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引用次数: 0
High-entropy catalysts for electrochemical water-electrolysis of hydrogen evolution and oxygen evolution reactions 用于电化学水电解氢进化和氧进化反应的高熵催化剂
IF 3.1 4区 工程技术 Q3 ENERGY & FUELS Pub Date : 2023-08-20 DOI: 10.1007/s11708-023-0892-6
Simiao Sha, Riyue Ge, Ying Li, Julie M. Cairney, Rongkun Zheng, Sean Li, Bin Liu, Jiujun Zhang, Wenxian Li

High entropy materials (HEMs) have developed rapidly in the field of electrocatalytic water-electrolysis for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) due to their unique properties. In particular, HEM catalysts are composed of many elements. Therefore, they have rich active sites and enhanced entropy stability relative to single atoms. In this paper, the preparation strategies and applications of HEM catalysts in electrochemical water-electrolysis are reviewed to explore the stabilization of HEMs and their catalytic mechanisms as well as their application in support green hydrogen production. First, the concept and four characteristics of HEMs are introduced based on entropy and composition. Then, synthetic strategies of HEM catalysts are systematically reviewed in terms of the categories of bottom-up and top-down. The application of HEMs as catalysts for electrochemical water-electrolysis in recent years is emphatically discussed, and the mechanisms of improving the performance of electrocatalysis is expounded by combining theoretical calculation technology and ex-situ/in situ characterization experiments. Finally, the application prospect of HEMs is proposed to conquer the challenges in HEM catalyst fabrications and applications.

高熵材料(HEM)因其独特的性质,在电催化水电解氧气进化反应(OER)和氢气进化反应(HER)领域发展迅速。特别是,HEM 催化剂由多种元素组成。因此,与单原子相比,它们具有丰富的活性位点和更强的熵稳定性。本文综述了 HEM 催化剂的制备策略和在电化学水-电解中的应用,探讨了 HEM 的稳定性、催化机理及其在支持绿色制氢中的应用。首先,介绍了基于熵和组成的 HEM 的概念和四个特征。然后,从自下而上和自上而下两方面系统地综述了 HEM 催化剂的合成策略。重点讨论了近年来 HEMs 作为电化学水电解催化剂的应用,并结合理论计算技术和原位/原位表征实验,阐述了 HEMs 提高电催化性能的机理。最后,提出了 HEMs 的应用前景,以应对 HEM 催化剂制造和应用中的挑战。
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引用次数: 0
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