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A review of anodic catalysts and their application in (non-)Kolbe electrocatalytic decarboxylation of carboxylic acids 阳极催化剂及其在(非)Kolbe电催化羧酸脱羧反应中的应用综述
IF 6 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2023-04-24 DOI: 10.1016/j.crcon.2023.04.004
Shichun Wang , Dezhang Ren , Yueying Du , Mengjie Zhang , Nahui Zhang , Yaguang Sun , Zhibao Huo

Biomass, as the exclusive and abundant organic resources, is considered to be the promising renewable resource. Carboxylic acids are one of the many compounds that can be obtained from raw biomass. Decarboxylation of carboxylic acids into fuels and chemicals via electrochemical method at mild reaction condition has been studied for many years. The (non-)Kolbe reaction, one of the oldest organic electrochemical reactions, is the decarboxylation of carboxylic acids to produce alkanes, alcohols, esters, etc. And electrode materials influence the production of electrocatalytic decarboxylation products from carboxylic acids. Therefore, this work mainly reviews the recent advances in applications of anodic materials for (non-)Kolbe electrocatalytic decarboxylation of carboxylic acids. It discusses the reaction mechanism of (non-) Kolbe electrolytic reaction, and the electrocatalytic oxidation of carboxylic acid using different electrodes and electrolytic systems to synthesize fuels and chemicals. Also, various types of electrode catalysts, such as Pt-based catalysts, C-based catalysts, and other catalysts, are introduced in detail. Finally, the challenges and future trends of the (non-)Kolbe reaction of carboxylic acids are presented. This review found that platinum-based electrocatalysts proved to be the most promising catalysts at present. And in recent years, a variety of synthesis methods have been developed to synthesize small size and high-performance noble metal based amorphous catalysts. Another approach is to study catalysts without platinum electricity, such as Ru, Ir, Ti and carbon materials. The review is helpful in understanding and know the anodic materials and their application in (non-)Kolbe electrocatalytic decarboxylation of carboxylic acids for the readers.

生物质作为一种独特而丰富的有机资源,被认为是一种很有前途的可再生资源。羧酸是可以从原料生物质中获得的许多化合物之一。在温和反应条件下,利用电化学方法将羧酸脱羧转化为燃料和化学品已经进行了多年的研究。(非)Kolbe反应是羧酸脱羧生成烷烃、醇、酯等的反应,是最古老的有机电化学反应之一。电极材料影响羧酸电催化脱羧产物的生产。因此,本文主要综述了近年来阳极材料在(非)Kolbe电催化羧酸脱羧中的应用进展。讨论了(非)Kolbe电解反应的反应机理,以及采用不同电极和电解体系对羧酸进行电催化氧化合成燃料和化学品。此外,还详细介绍了各种类型的电极催化剂,如pt基催化剂、c基催化剂等。最后,提出了羧酸(非)Kolbe反应的挑战和未来发展趋势。本文综述了铂基电催化剂是目前最具发展前景的催化剂。近年来,人们发展了多种合成方法来合成小尺寸、高性能的贵金属基非晶催化剂。另一种方法是研究不含铂电的催化剂,如Ru、Ir、Ti和碳材料。本文的综述有助于读者理解和认识阳极材料及其在(非)Kolbe电催化羧酸脱羧中的应用。
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引用次数: 0
Green synthesis of magnetically separable and reusable Fe3O4/Cdots nanocomposites photocatalyst utilizing Moringa oleifera extract and watermelon peel for rapid dye degradation 利用辣木提取物和西瓜皮绿色合成磁性可分离、可重复使用的Fe3O4/Cdots纳米复合光催化剂,用于快速降解染料
IF 6 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2023-04-14 DOI: 10.1016/j.crcon.2023.04.003
Emi Kurnia Sari , Rivaldo Marsel Tumbelaka , Harlina Ardiyanti , Nurul Imani Istiqomah , Chotimah , Edi Suharyadi

This study focused on green-synthesized magnetite/carbon dots nanocomposites (GS-Fe3O4/Cdots) utilizing Moringa oleifera leaf extract and watermelon peel waste for rapid degradation of methylene blue (MB) dye. Co-precipitation and hydrothermal method were used to synthesize GS-Fe3O4 and Cdots, respectively. In addition, the sonication method was used to link Cdots on Fe3O4 surface. X-ray diffraction spectrum of GS-Fe3O4/Cdots inform the cubic inverse spinel and has crystallite size in the range of 10.1–7.2 nm. The crystallite size also decreased with the increase of Cdots concentration. The transmission electron microscope showed the most uniform size of nanocomposites at around 13.4 nm. The functional group of Fe-O was detected on the nanocomposites, proof that Fe3O4 still exists after fabrication. The presence of C = C, C-O, and C-O-C also indicates the existence of Cdots on the surface of Fe3O4. The addition of Cdots affected the saturation magnetization and coercivity value in the range of 29.2 – 38.3 emu/g and 59–65 Oe, respectively, which showed a good magnetic properties. As an organic dye, MB was used for a photocatalytic process under UV irradiation. The degradation efficiency was raised to 98% for 30 min photocatalytic process. The magnetically separable capability makes nanocomposites could be recycled and reused three times with high degradation. Furthermore, GS-Fe3O4/Cdots potential as a low-cost and environmentally friendly reusable photocatalyst for rapid wastewater degradation.

本研究利用辣木叶提取物和西瓜皮废料快速降解亚甲基蓝(MB)染料,制备了绿色合成的磁铁矿/碳点纳米复合材料(GS-Fe3O4/Cdots)。采用共沉淀法和水热法分别合成了GS-Fe3O4和Cdots。此外,还采用超声处理方法在Fe3O4表面连接Cdots。GS-Fe3O4/Cdots的X射线衍射光谱显示出立方反尖晶石,其晶粒尺寸在10.1–7.2 nm之间。晶粒尺寸也随着Cdots浓度的增加而减小。透射电子显微镜显示,纳米复合材料的尺寸在13.4 nm左右最均匀。在纳米复合材料上检测到Fe-O的官能团,证明Fe3O4在制备后仍然存在。C=C、C-O和C-O-C的存在也表明在Fe3O4表面上存在Cdots。Cdots的加入对饱和磁化强度和矫顽力的影响范围分别为29.2–38.3 emu/g和59–65 Oe,表现出良好的磁性。MB作为一种有机染料,在紫外线照射下用于光催化过程。光催化30min,降解效率提高到98%。纳米复合材料具有可磁性分离的性能,可重复使用三次,降解率高。此外,GS-Fe3O4/Cdots有潜力成为一种低成本、环保的可重复使用的光催化剂,用于快速降解废水。
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引用次数: 0
A green route for hydrogen production from alkaline thermal treatment (ATT) of biomass with carbon storage 生物质储碳碱性热处理制氢的绿色途径
IF 6 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2023-04-12 DOI: 10.1016/j.crcon.2023.04.001
Guojie Liu , Zexue Du , Houfang Lu , Jianli Zeng , Kejing Wu , Bin Liang

Hydrogen, a green energy carrier, is one of the most promising energy sources. However, it is currently mainly produced from depleting fossil fuels with high carbon emissions, which has serious negative effects on the economy and environment. To address this issue, sustainable hydrogen production from bio-energy with carbon capture and storage (HyBECCS) is an ideal technology to reduce global carbon emissions while meeting energy demand. This review presents an overview of the latest progress in alkaline thermal treatment (ATT) of biomass for hydrogen production with carbon storage, especially focusing on the technical characteristics and related challenges from an industrial application perspective. Additionally, the roles of alkali and catalyst in the ATT process are critically discussed, and several aspects that have great influences on the ATT process, such as biomass types, reaction parameters, and reactors, are expounded. Finally, the potential solutions to the general challenges and obstacles to the future industrial-scale application of ATT of biomass for hydrogen production are proposed.

氢是一种绿色能源载体,是最有前途的能源之一。然而,目前它主要来自高碳排放的化石燃料的消耗,这对经济和环境有严重的负面影响。为了解决这一问题,利用生物能源与碳捕获和储存(HyBECCS)进行可持续制氢是一种理想的技术,可以在满足能源需求的同时减少全球碳排放。本文综述了生物质碱性热处理储碳制氢技术的最新进展,着重从工业应用的角度分析了其技术特点和面临的挑战。此外,对碱和催化剂在ATT工艺中的作用进行了批判性讨论,并对生物质类型、反应参数、反应器等对ATT工艺影响较大的几个方面进行了阐述。最后,提出了潜在的解决方案,以解决未来工业规模应用生物质制氢的一般挑战和障碍。
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引用次数: 1
Utilization of fruit waste for H2-rich syngas production via steam co-gasification with brown coal 利用水果废弃物与褐煤蒸汽共气化生产富H2合成气
IF 6 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2023-04-12 DOI: 10.1016/j.crcon.2023.04.002
Aisikaer Anniwaer , Nichaboon Chaihad , Aghietyas Choirun Az Zahra , Irwan Kurnia , Yutaka Kasai , Suwadee Kongparakul , Chanatip Samart , Katsuki Kusakabe , Abuliti Abudula , Guoqing Guan

In this work, to efficiently utilize waste fruit and low-rank coal for the hydrogen (H2)-rich syngas production, steam co-gasification of banana peel (BP) and brown coal (BC) was studied in a fixed-bed reactor. The results showed that the gasification rate of BC was highly enhanced after mixing it with BP and the obvious synergistic effect was observed in all investigated three mixing weight ratios (i.e., 1:1, 1:4, 4:1), resulting in a higher carbon conversion as well as a H2-rich gas production yield for the co-gasification. However, the extent of promotion by synergistic effect was affected by the reaction temperature, mixing ratio, and steam amount. It was found that the high potassium (K) species content in the BP provided the catalytic effect not only on water–gas shift reaction but also on tar reforming/cracking, thereby enhancing the gasification of BC. In addition, it is confirmed that steam should be an important factor to promote the synergistic effect and H2-rich gas production.

为了高效利用废水果和低阶煤生产富氢合成气,在固定床反应器上对香蕉皮(BP)和褐煤(BC)的蒸汽共气化进行了研究。结果表明,BC与BP混合后气化率显著提高,且3种混合质量比(1:1、1:4、4:1)均表现出明显的协同效应,使得共气化的碳转化率和富h2产气量均有所提高。而协同效应的促进程度受反应温度、混合比和蒸汽量的影响。结果表明,BP中钾(K)的高含量不仅对水煤气转换反应有催化作用,而且对焦油重整/裂化也有催化作用,从而促进了BC的气化。此外,还证实了蒸汽是促进协同效应和富h2产气的重要因素。
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引用次数: 1
Green Synthesize of Magnetically Separable and Reusable Fe3O4/Cdots Nanocomposites Photocatalyst utilizing Moringa Oleifera Extract and Watermelon Peel for Rapid Dye Degradation 利用辣木提取物和西瓜皮绿色合成磁性可分离、可重复使用的Fe3O4/Cdots纳米复合光催化剂用于快速降解染料
IF 6 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2023-04-01 DOI: 10.1016/j.crcon.2023.04.003
Emi Kurnia Sari, Rivaldo Marsel Tumbelaka, H. Ardiyanti, Nurul Imani Istiqomah, Chotimah, E. Suharyadi
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引用次数: 5
Studies on the co-metabolism of glucose and glycerol in the fungus Umbelopsis isabellina 葡萄糖和甘油在深叶伞藻真菌中的共代谢研究
IF 6 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2023-03-25 DOI: 10.1016/j.crcon.2023.03.008
Panagiotis Dritsas, George Aggelis

Over the past few years, it is observed an increased interest for oleaginous microorganisms in the perspective to produce microbial oils of great commercial interest through the consumption of low/zero cost substrates. In this paper, the physiology of the fungus Umbelopsis isabellina growing on blends of glycerol and glucose was investigated. In all experiments the fungus completely consumed glucose and produced satisfactory quantities of biomass containing reserve lipids in high percentages. However, glycerol concentration in the growth medium was negatively correlated to glucose assimilation rate, mainly during the balanced-growth phase. Nevertheless, at high initial concentrations, glycerol was partially consumed and seemed to contribute positively to the suppression of lipid degradation. Following the discovery of this complex regulatory mechanism regarding glucose and glycerol co-assimilation, the activity of three key-enzymes namely aldolase, glycerol kinase and glycerol dehydrogenase, which are implicated in glycerol and glucose assimilation, was investigated. The experiments revealed a clear preference of the fungus for glucose over glycerol. On the other hand, storage polysaccharides are degraded instead of storage lipid at the late oleaginous phase for maintenance purpose. These new biochemical features will enable the design of appropriate growth media for the co-fermentation of these two substrates by U. isabellina with the aim to maximize lipid accumulation.

在过去的几年里,人们观察到对含油微生物越来越感兴趣,因为通过消耗低成本/零成本的底物来生产具有巨大商业价值的微生物油。本文研究了在甘油和葡萄糖混合培养基上生长的黄曲霉的生理特性。在所有实验中,真菌完全消耗了葡萄糖,并产生了令人满意的生物量,其中含有高百分比的储备脂质。然而,生长培养基中的甘油浓度与葡萄糖同化率呈负相关,主要是在平衡生长阶段。然而,在高初始浓度下,甘油被部分消耗,并且似乎对抑制脂质降解有积极贡献。在发现葡萄糖和甘油共同化的复杂调节机制后,研究了与甘油和葡萄糖同化有关的三种关键酶,即醛缩酶、甘油激酶和甘油脱氢酶的活性。实验表明,真菌对葡萄糖的偏好明显高于甘油。另一方面,在含油后期,为了维持目的,储存多糖而不是储存脂质被降解。这些新的生物化学特征将使褐黄菌能够为这两种底物的共同发酵设计合适的生长培养基,以最大限度地增加脂质积累。
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引用次数: 0
Carbon materials in electrocatalytic oxidation systems for the treatment of organic pollutants in wastewater: A review 电催化氧化系统中碳材料处理废水中有机污染物的研究进展
IF 6 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2023-03-21 DOI: 10.1016/j.crcon.2023.03.006
Xintong Duan , Dezhang Ren , Shichun Wang , Mengjie Zhang , Yaguang Sun , Shujing Sun , Zhibao Huo , Nahui Zhang

Carbon materials are widely used as catalysts in electrocatalytic oxidative (EO) degradation of wastewater due to their large specific surface area and low cost. Carbon materials can also be used as catalyst carriers for EO reactions due to their ease of functionalization with other heteroatoms and metals/metal oxides. To improve the catalytic activity and current efficiency of carbon materials, modifying the structural and physicochemical properties of conventional carbon materials are common improvement method. This review briefly outlines the recent research progress of carbon materials in EO for organic pollutants degradation. It also discusses the modification strategies and corresponding electrocatalytic properties of various carbon materials (carbon nanomaterials and porous carbon materials), and explores the EO mechanism. Finally, some summaries of the remaining challenges and future developments of carbon materials in the field of electrocatalysis are given.

碳材料具有比表面积大、成本低等优点,在电催化氧化降解废水中得到了广泛的应用。由于碳材料易于与其他杂原子和金属/金属氧化物官能化,因此也可以用作EO反应的催化剂载体。为了提高碳材料的催化活性和电流效率,对常规碳材料的结构和理化性质进行改性是常用的改进方法。本文综述了近年来碳材料在EO中降解有机污染物的研究进展。讨论了各种碳材料(碳纳米材料和多孔碳材料)的改性策略和相应的电催化性能,并探讨了电催化机理。最后,对碳材料在电催化领域存在的挑战和未来的发展进行了总结。
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引用次数: 4
Hydrogen storage by liquid organic hydrogen carriers: Catalyst, renewable carrier, and technology – A review 液态有机氢载体储氢:催化剂、可再生载体和技术——综述
IF 6 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2023-03-21 DOI: 10.1016/j.crcon.2023.03.007
Chenyang Chu, Kai Wu, Bingbing Luo, Qi Cao, Huiyan Zhang

Hydrogen has attracted widespread attention as a carbon-neutral energy source, but developing efficient and safe hydrogen storage technologies remains a huge challenge. Recently, liquid organic hydrogen carriers (LOHCs) technology has shown great potential for efficient and stable hydrogen storage and transport. This technology allows for safe and economical large-scale transoceanic transportation and long-cycle hydrogen storage. In particular, traditional organic hydrogen storage liquids are derived from nonrenewable fossil fuels through costly refining procedures, resulting in unavoidable environmental contamination. Biomass holds great promise for the preparation of LOHCs due to its unique carbon-balance properties and feasibility to manufacture aromatic and nitrogen-doped compounds. According to recent studies, almost 100% conversion and 92% yield of benzene could be obtained through advanced biomass conversion technologies, showing great potential in preparing biomass-based LOHCs. Overall, the present LOHCs systems and their unique applications are introduced in this review, and the technical paths are summarized. Furthermore, this paper provides an outlook on the future development of LOHCs technology, focusing on biomass-derived aromatic and N-doped compounds and their applications in hydrogen storage.

氢作为一种碳中性能源受到了广泛关注,但开发高效、安全的储氢技术仍然是一个巨大的挑战。近年来,液态有机氢载体(lohc)技术在高效、稳定的储氢和输氢方面显示出巨大的潜力。该技术可实现安全、经济的大规模跨洋运输和长周期储氢。特别是,传统的有机储氢液体是通过昂贵的精炼程序从不可再生的化石燃料中提取的,导致不可避免的环境污染。生物质由于其独特的碳平衡特性和制备芳香族和氮掺杂化合物的可行性,在制备lohc方面具有很大的前景。根据最近的研究,通过先进的生物质转化技术,苯的转化率几乎可以达到100%,收率可以达到92%,在制备生物质基lohc方面显示出巨大的潜力。综述了现有的lohc系统及其独特的应用,并对其技术路径进行了总结。展望了lohc技术的未来发展,重点关注生物质衍生芳香族化合物和n掺杂化合物及其在储氢领域的应用。
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引用次数: 10
Role of oxygen species and active phase of CuCeZrOx prepared with bacterial cellulose for toluene catalytic oxidation 细菌纤维素制备CuCeZrOx在甲苯催化氧化中的作用及活性相
IF 6 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2023-03-14 DOI: 10.1016/j.crcon.2023.03.005
Chenhang Zhang , Chenchen Zhao , Running Kang , Qinglan Hao , Baojuan Dou , Feng Bin

The present study investigates the active phases and the role of oxygen species in the toluene oxidation process over CuCeZrOx catalysts prepared with bacterial cellulose (BC), and compares them with nitric acid pickling CuCeZrOx-BC(H) and CeZrOx-BC catalysts. The investigation is carried out using in-situ DRIFT, O2-TPD, H2-TPR, XRD, and TEM techniques. Our findings suggest that dispersed CuO species on the catalyst surface, Cu-Ce-Zr-O, and Ce-Zr-O solid solutions are active for toluene oxidation over CuCeZrOx-BC, with corresponding activities decreasing successively. The in-situ DRIFT results demonstrate that gaseous oxygen facilitates the chemisorption of toluene on active oxygen species, forming benzoyl oxide species and partially oxidizing the absorbed intermediates to benzyl alcohol at room temperature. Furthermore, lattice oxygen is experimentally found to be involved in the deep oxidation of toluene, and the lattice oxygen present in dispersed CuO species dominates the toluene oxidation process over CuCeZrOx-BC.

本研究研究了细菌纤维素(BC)制备的CuCeZrOx催化剂上的活性相及其氧在甲苯氧化过程中的作用,并将其与硝酸酸洗CuCeZrOx-BC(H)和CeZrOx-BC催化剂进行了比较。利用原位DRIFT、O2-TPD、H2-TPR、XRD和TEM技术进行了研究。我们的研究结果表明,分散在催化剂表面的CuO物种、Cu-Ce-Zr-O和Ce-Zr-O固溶体对CuCeZrOx-BC上的甲苯氧化具有活性,相应的活性依次降低。原位DRIFT结果表明,气态氧促进甲苯在活性氧物种上的化学吸附,形成苯甲酰氧化物物种,并在室温下将吸收的中间体部分氧化为苯甲醇。此外,实验发现晶格氧参与甲苯的深度氧化,并且存在于分散的CuO物种中的晶格氧在甲苯氧化过程中比CuCeZrOx BC占主导地位。
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引用次数: 0
Hydrothermal pretreatment of protein-rich substrate: Modified physicochemical properties and consequent responses in its anaerobic digestion 富蛋白底物的水热预处理:对其厌氧消化的理化性质及其后续反应的修改
IF 6 3区 环境科学与生态学 Q2 ENERGY & FUELS Pub Date : 2023-03-01 DOI: 10.1016/j.crcon.2022.10.001
Fa Qiao , Guangyi Zhang , Jie Fan , Hang Zhang , Bowen Shi , Jiancheng Yang , Jianling Zhang , Zhennan Han

Wasted tofu rich in protein was subject to hydrothermal pretreatment (HTPT) under different conditions (at 120, 140, 160 and 180 ℃; for 0, 30, 60 and 90 min) followed by biochemical methane potential (BMP) tests, and 140 ℃ and 0 min were found to be respectively the best temperature and duration for HTPT of tofu in terms of its biogas production. Under the under the optimal conditions (140 ℃, 0 min) the accumulative methane yield reached up to 510.9 mL·(gVS)-1, which was 26.98 % higher than that without HTPT (402.3 mL·(gVS)-1). The start-up process of continuous anerobic digestion (AD) of the tofu before and after hydrothermal treated (HT) at the optimal HTPT conditions (140 ℃, 0 min) was examined, to investigate and compare how their consequent AD responded to HTPT. It was found that, for start-up of continuous AD, the HT tofu delivered more balanced nutrients and thus led to more stable AD and quicker biogas production. Unavoidably, HTPT generated products refractory to biodegradation, to slightly decrease the total biogas production. During AD of HT tofu some weak ammonia-tolerant microbes, such as methylotrophic methanogens, survived and played indispensable roles. Analyses of living microbial community structure indicated that, some hydrolytic acidification bacteria intolerant to ammonia nitrogen (such as Proteobacteria) were always active and appeared at high proportion. The viable methylotrophic methanogens, e. g. RumEn M2, took obvious responsibilities in start-up of the AD for HT tofu.

对富含蛋白质的废弃豆腐在不同条件下(120、140、160和180℃;0、30、60和90min)进行水热预处理,然后进行生化甲烷电位(BMP)测试,发现140℃和0min分别是豆腐产生沼气的最佳水热处理温度和时间。在最佳条件(140℃,0min)下,累积甲烷产量高达510.9mL·(gVS)-1,比不加HTPT的(402.3mL·(g VS)-1)高26.98%,以调查和比较他们随后的AD对HTPT的反应。研究发现,对于连续AD的启动,HT豆腐提供了更平衡的营养,从而导致更稳定的AD和更快的沼气生产。不可避免的是,HTPT产生了难以生物降解的产物,从而略微降低了沼气的总产量。在耐高温豆腐的AD过程中,一些弱耐氨微生物,如甲基营养产甲烷菌,得以存活并发挥了不可或缺的作用。活菌群落结构分析表明,一些对氨氮不耐受的水解酸化菌(如变形杆菌)始终具有较高的活性,并以较高的比例出现。有活力的甲基营养产甲烷菌,如RumenM2,在HT豆腐AD的启动过程中承担了明显的责任。
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引用次数: 1
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