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Effect of Shell Thickness on the Properties of Multi-Pd Cores-Hollow Carbon Shell Catalyst mPd@HCS 壳层厚度对多钯芯-空心碳壳催化剂性能的影响mPd@HCS
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-07-04 DOI: 10.1007/s10563-022-09362-y
Feifei Hu, Chengbing Fu, Chenchen Zhao, Peng Liu, Wei Tian, Bo Chen, Hongyan Pan, Qian Lin

Traditional catalysts with one core and one shell structure have few active sites and shell structure parameters are difficult to be regulated. In order to solve these two problems, it is presented herein a multi-Pd-core and porous carbon shell catalyst mPd@HCS, where multiple Pd nuclei provide more active sites for the reaction, the shell structure parameters are tuned by the adjustment of shell thickness, and the influence of shell thickness on the performance of H2O2 direct synthesis was mainly investigated. The results showed that the selectivity and yield of H2O2 changed volcanically with the increase of carbon crust thickness because of the compromise between reactants diffusion and product degradation, and the selectivity (87%) and productivity (1938 mmol gPd−1 h−1) of the sample with middle shell thickness (10.18 nm) were the highest.

传统的一核一壳结构催化剂活性位点少,壳结构参数难以调控。为了解决这两个问题,本文提出了一种多钯核多孔碳壳催化剂mPd@HCS,其中多钯核为反应提供了更多的活性位点,通过调整壳层厚度来调整壳层结构参数,并主要研究了壳层厚度对H2O2直接合成性能的影响。结果表明,H2O2的选择性和产率随碳壳厚度的增加呈火山状变化,这是由于反应物扩散和产物降解之间的折衷,其中,中壳厚度(10.18 nm)样品的选择性(87%)和产率(1938 mmol gPd−1 h−1)最高。
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引用次数: 0
Review: Graphite Phase Carbon Nitride Photo-Fenton Catalyst and its Photocatalytic Degradation Performance for Organic Wastewater 综述:石墨相氮化碳光fenton催化剂及其对有机废水的光催化降解性能
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-06-20 DOI: 10.1007/s10563-022-09363-x
Jingpeng Luo, Xu Du, Qingying Ye, Dong Fu

The catalytic properties and applications of Fenton and Fenton-like catalysts based on graphitic carbon nitride (g-C3N4) are reviewed. Compared with semiconductor photocatalytic, the synergistic system of photocatalysis and Fenton-like oxidation has a stronger ability to degrade organic wastewater, but there are still some shortcomings, such as high recombination rate of photogenerated carriers and serious agglomeration of metals on the catalyst surface, and its catalytic performance still needs to be further improved. The development of heterogeneous photo-Fenton-like catalysts based on g-C3N4 and their Fenton-like mechanism will be the focus of future research.

综述了氮化石墨碳(g-C3N4)基Fenton及类Fenton催化剂的催化性能及应用。与半导体光催化相比,光催化与类芬顿氧化协同体系对有机废水的降解能力更强,但仍存在光生载体复合率高、金属在催化剂表面团聚严重等缺点,其催化性能有待进一步提高。基于g-C3N4的非均相光fenton类催化剂的开发及其fenton类机理将是未来研究的重点。
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引用次数: 3
Wild Olive Oil as a Novel and Sustainable Feedstock for Biodiesel Production: Overviewed Various Feedstock, Methodologies and Reaction Mechanisms of Different Catalysts 野生橄榄油作为生物柴油生产的新型可持续原料:各种原料、方法和不同催化剂的反应机理综述
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-06-03 DOI: 10.1007/s10563-022-09361-z
Ihtisham Wali Khan, Abdul Naeem, Muhammad Farooq, Tahira Mahmood, Tooba Saeed, Fouzia Parveen, Tabassum Malik

The over-consumption of petroleum fuel due to the progressive increase in population, transportation, industrialization, modernization as well as improvement in the lifestyle of the society leads to the fast declining of non-renewable resources. Therefore, it is important to discover low cost, environmentally friendly and sustainable surrogates of petroleum fuels. In this regard, biodiesel production is one of the gorgeous solutions for the research community. Contrary to the benefits, the high cost of the biodiesel is the main disadvantage, greatly reliant on the feedstock. In this sense, wild olive oil was explored for the first time as a suitable and novel feedstock for biodiesel technology development. The fatty acid composition was identified by GC–MS analysis whereas various physiochemical properties were determined by ASTM and EN methods. Furthermore, this review paper conveys a detailed overview of biodiesel production technologies, various generation feedstocks and types of catalyst along with their plausible mechanism.

由于人口、交通、工业化、现代化以及社会生活方式的不断提高,石油燃料的过度消耗导致了不可再生资源的快速减少。因此,寻找低成本、环保、可持续的石油燃料替代品具有重要意义。在这方面,生物柴油生产是研究界的华丽解决方案之一。与优点相反,生物柴油的主要缺点是成本高,严重依赖原料。从这个意义上说,野生橄榄油首次被探索为一种适合生物柴油技术发展的新型原料。脂肪酸组成采用气相色谱-质谱法鉴定,理化性质采用ASTM和EN法测定。此外,本文还详细介绍了生物柴油的生产技术、各种生产原料和催化剂类型及其可能的机理。
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引用次数: 0
Catalytic Oxidation of Ethyl Lactate to Ethyl Pyruvate over Au-Based Catalyst Using Authentic Air as Oxidant 真实空气作氧化剂在金基催化剂上催化氧化乳酸乙酯制丙酮酸乙酯
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-05-21 DOI: 10.1007/s10563-022-09359-7
Shiyao Lu, Jian Zhang, Zhiyi Wu, Zerui Su, Jianbin Huang, Yehao Liang, Feng-Shou Xiao

Highly dispersed Au nanoparticles supported on Ni–Al mixed metal oxides (Au/NiAl-MMO) were prepared by a facile method, which is significantly efficient for the aerobic oxidation of ethyl lactate using authentic air as the oxidant, achieving 72.6% ethyl lactate conversion and 88.3% selectivity to ethyl pyruvate at 240 °C in a continuous fixed-bed reactor. The catalyst retained its catalytic performance during a long-term stability test. Characterization and experimental studies on the kinetic dependence sequence of the reactants and elementary reaction steps confirmed that the Au/NiAl-MMO catalyst followed the Mars–van Krevelen mechanism, with the activation of O2 as the elementary step. The quasi in situ X-ray photoelectron spectroscopy spectra demonstrated that the active sites in the Au/NiAl-MMO catalyst were Au nanoparticles. This work may provide a novel technique for developing more efficient supported metal catalysts for the aerobic oxidation of ethyl lactate using authentic air as the oxidant.

Graphical abstract

Highly dispersed Au nanoparticle catalyst was facilely prepared for the efficient catalytic oxidation of ethyl lactate with authentic air.

采用简便方法制备了负载在Ni-Al混合金属氧化物(Au/NiAl-MMO)上的高度分散的Au纳米颗粒,该纳米颗粒在真实空气为氧化剂的条件下对乳酸乙酯的好氧氧化效果显著,在240℃的连续固定床反应器中乳酸乙酯转化率为72.6%,丙酮酸乙酯选择性为88.3%。该催化剂在长期稳定性试验中保持了其催化性能。对反应物和基本反应步骤的动力学依赖顺序进行表征和实验研究,证实Au/NiAl-MMO催化剂遵循Mars-van Krevelen机理,以O2活化为基本反应步骤。准原位x射线光电子能谱分析表明,Au/NiAl-MMO催化剂的活性位点为Au纳米粒子。本研究为开发以真实空气为氧化剂的负载型金属催化剂制备乳酸乙酯的好氧反应提供了一种新技术。摘要制备了分散的金纳米颗粒催化剂,用于乳酸乙酯在真实空气中的高效催化氧化。
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引用次数: 0
2-Pyridyl-benzimidazole-Pd(II)/Pd(0) Supported on Magnetic Mesoporous Silica: Aerobic Oxidation of Benzyl Alcohols/Benzaldehydes and Reduction of Nitroarenes 磁性介孔二氧化硅负载的2-吡啶-苯并咪唑-Pd(II)/Pd(0):苯甲醇/苯甲醛的好氧氧化和硝基芳烃的还原
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-05-10 DOI: 10.1007/s10563-022-09360-0
Mohammad Sajedi, Yagoub Mansoori, Ayat Nuri, Somayeh Fekri, Dolores Esquivel, Mª Angeles Navarro

2-(2-Pyridyl)benzimidazole (PyBzIm) was supported onto magnetic mesoporous silica, Fe3O4@SiO2@SBA-15 via the click chemistry. The supported ligand was treated with Na2PdCl4 in methanol to afford Fe3O4@SiO2@SBA-PyBzIm-Pd(II) as a magnetically retrievable supported catalyst. The catalyst was fully characterized by conventional methods. X-ray photoelectron spectroscopy (XPS) studies confirmed some C = N nitrogen atoms interact with palladium in the + 2 oxidation state. The prepared catalyst was found to catalyze the aerobic oxidation of benzyl alcohols and benzaldehydes to the corresponding benzoic acids, and excellent conversions were obtained. The magnetic catalyst showed a very low metal leaching (3.9%) in the first run. Fe3O4@SiO2@SBA-PyBzIm-Pd(II) was then treated with aqueous NaBH4 to give Fe3O4@SBA-PyBzIm-Pd(0). The obtained catalyst was found to catalyze the transfer hydrogenation of nitroarenes to the corresponding anilines in the presence of hydrazine, and excellent yields were obtained. The prepared catalysts present an excellent recycling efficiency over seven consecutive runs without significant loss of catalyst reactivity.

Graphical abstract

通过点击化学将2-(2-吡啶基)苯并咪唑(PyBzIm)负载在磁性介孔二氧化硅Fe3O4@SiO2@SBA-15上。负载配体用Na2PdCl4在甲醇中处理,得到Fe3O4@SiO2@ sba - pybzem - pd (II)作为磁性可回收负载催化剂。用常规方法对催化剂进行了表征。x射线光电子能谱(XPS)研究证实了一些C = N的氮原子与钯以+ 2氧化态相互作用。所制备的催化剂能催化苯甲醇和苯甲醛的好氧氧化生成苯甲酸,并取得了良好的转化率。在第一次运行中,磁性催化剂的金属浸出率很低(3.9%)。Fe3O4@SiO2@SBA-PyBzIm-Pd(II)用NaBH4水溶液处理得到Fe3O4@SBA-PyBzIm-Pd(0)。结果表明,该催化剂能在肼存在下催化硝基芳烃的转移加氢反应生成相应的苯胺,收率较高。制备的催化剂在连续七次运行中表现出优异的回收效率,而催化剂的反应性没有明显损失。图形抽象
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引用次数: 4
Trimetallic PtTiMg Alloy Nanoparticles with High Activity for Efficient Electrocatalytic Ethanol Oxidation 高效电催化乙醇氧化的三金属PtTiMg合金纳米颗粒
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-04-04 DOI: 10.1007/s10563-022-09355-x
Guangquan Liu, Liping Peng, Long Fan, Jin Wang, Yajun Fu, Linhong Cao, Weidong Wu

Although nanostructures based on noble metal alloys are widely used in the anode catalysts of direct ethanol fuel cells, their commercialization remains a remarkable challenge due to their high cost and poor durability. We describe the successful synthesis of trimetallic PtTiMg alloy nanoparticles with adjustable composition using a simple one-step three-target magnetron co-sputtering method. Various physical characterization and electrochemical methods were used to investigate the structure/composition and electrochemical properties of the obtained PtTiMg alloy catalysts toward ethanol oxidation reaction (EOR). The PtTiMg alloy catalyst demonstrated excellent electrocatalytic activity and high durability when the Mg content was 2.76%, (after 3000 cycles, retained 91% of its electrochemical surface area). Furthermore, the electrochemically active surface area and peak current density of the PtTiMg alloy catalyst are 1.5 and 0.8 times higher than those of the commercial pure Pt catalyst, respectively. Furthermore, the long-term strong acid immersion test demonstrated that the PtTiMg alloy catalysts retain high electrocatalytic activity in harsh environments, demonstrating the potential application of the obtained PtTiMg alloy catalysts for EOR.

尽管基于贵金属合金的纳米结构广泛应用于直接乙醇燃料电池的阳极催化剂,但由于其成本高且耐久性差,其商业化仍然是一个显着的挑战。我们描述了用简单的一步三靶磁控共溅射方法成功合成了具有可调成分的三金属PtTiMg合金纳米颗粒。采用各种物理表征和电化学方法对制备的PtTiMg合金乙醇氧化反应催化剂的结构组成和电化学性能进行了研究。当Mg含量为2.76%时,PtTiMg合金催化剂表现出优异的电催化活性和较高的耐久性(循环3000次后,其电化学表面积保留91%)。此外,PtTiMg合金催化剂的电化学活性表面积和峰值电流密度分别是商用纯Pt催化剂的1.5倍和0.8倍。此外,长期强酸浸泡试验表明,PtTiMg合金催化剂在恶劣环境下仍保持较高的电催化活性,证明了所制备的PtTiMg合金催化剂在提高采收率方面的潜在应用前景。
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引用次数: 0
Catalytic Transesterification of Coconut Oil in Biodiesel Production: A Review 椰子油催化酯交换技术在生物柴油生产中的研究进展
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-03-30 DOI: 10.1007/s10563-022-09358-8
Aisyah Fathiah Ahmad, Nursyamimi Zulkurnain, Salmiah Jamal Mat Rosid, Azman Azid, Azizah Endut, Susilawati Toemen, Salwani Ismail, Wan Nazwanie Wan Abdullah, Siti Maisarah Aziz, Nurulhuda Mohammed Yusoff, Sarina Mat Rosid, Nur Atiqah Nasir

Biodiesel is one of the renewable energy (RE) sources that has received much interest due to its promising properties. Recently, the use of coconut oil as biodiesel has caught the attention of many researchers. As a result, this paper presents a comprehensive overview of the current catalysts used to produce coconut oil biodiesel via the transesterification method.

Graphical Abstract

生物柴油是近年来备受关注的可再生能源之一。最近,使用椰子油作为生物柴油引起了许多研究人员的注意。因此,本文对目前用于酯交换法生产椰子油生物柴油的催化剂进行了全面的综述。图形抽象
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引用次数: 9
Effect of Co-catalyst CdS on the Photocatalytic Performance of ZnMoO4 for Hydrogen Production 助催化剂CdS对ZnMoO4制氢光催化性能的影响
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-03-18 DOI: 10.1007/s10563-022-09357-9
Ming Zheng, Bing Gao, Suwen Tang, Min Zhu, Liang Tang, Minghong Wu

Zinc molybdate (ZnMoO4), a layer perovskite material, has the advantages of high stability, excellent optical and charge properties. However, its high band gap and high electron–hole recombination efficiency limit its application in the photocatalytic reduction field like hydrogen production. In this study, we used CdS as a co-catalyst and successfully prepared CdS/ZnMoO4 composite photocatalysts with different loadings. The hydrogen evolution rate of CdS/ZnMoO4 reached 530.2 µmol h−1 g−1, which was approximately 11 and 100 times more than rates of pure CdS and ZnMoO4 under the same conditions, respectively. It is the presence of CdS that contributed to this improved performance, which acted as an electron acceptor to separate electrons and holes. Besides, a reasonable mechanism was provided based on photoelectrochemical characterizations. CdS loading greatly improved the hydrogen evolution performance of ZnMoO4 under visible light, providing a direction to improving the performance of perovskite based photocatalysts.

钼酸锌(ZnMoO4)是一种层状钙钛矿材料,具有稳定性高、光学性能和电荷性能优异等优点。但其高带隙和高电子空穴复合效率限制了其在制氢等光催化还原领域的应用。在本研究中,我们以CdS为助催化剂,成功制备了不同负载的CdS/ZnMoO4复合光催化剂。cd /ZnMoO4的析氢速率达到530.2µmol h−1 g−1,分别是纯cd和ZnMoO4的11倍和100倍。cd的存在有助于提高性能,它作为电子受体将电子和空穴分开。并基于光电化学表征给出了合理的机理。加载CdS大大提高了ZnMoO4在可见光下的析氢性能,为提高钙钛矿基光催化剂的性能提供了方向。
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引用次数: 2
Enhanced Catalytic Activity and SO2/H2O Tolerance for Selective Catalytic Reduction of NOx with NH3 over Titanate Nanotubes Supported MnOx–CeO2 Catalyst at Low Temperature 二氧化钛纳米管负载MnOx-CeO2催化剂在低温条件下NH3选择性催化还原NOx的活性和SO2/H2O耐受性增强
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-03-16 DOI: 10.1007/s10563-022-09356-w
Zhuping Jiang, Qiulin Wang, Yuzhou Cai

An environment-friendly selective catalytic reduction (SCR) catalyst with high catalytic activity and strong anti-poisoning performance at low temperature is strongly needed to achieve the wide application of low temperature NH3-SCR technology. Selection of appropriate carrier is one of the most important measures to improve catalytic activity as well as anti-poisoning capability of SCR catalyst. Manganese oxide-cerium oxide supported on traditional titanium dioxide (denoted as MnCe/TiO2) and titanate nanotubes (denoted as MnCe/TiNTs) were prepared by impregnation method and their catalytic activities towards NH3-SCR of NO were evaluated in flue gas with or without SO2 & H2O. The results indicate that TiNTs with optimum morphology and microstructure can be obtained when P25 TiO2 is hydrothermally treated at 130 °C for 24 h. Supporting MnOx–CeO2 composite on TiNTs not only enhances the catalytic activity at low temperature, but also improves N2 selectivity and widens active temperature window of catalyst. The main reason is the large specific surface area as well as the unique hollow tubular structure of TiNTs facilitates high dispersion of catalytic active components on the inner and outer walls of TiNTs, which enriches surface acid sites and surface reactive oxygen species to fulfill low temperature SCR reaction cycle. Moreover, TiNTs significantly enhances the SO2 & H2O tolerance of catalyst, for the competitive adsorption between SO2, H2O and reactants is alleviated and the deposition of ammonium sulphate or ammonium bisulphate becomes more difficult on MnCe/TiNTs catalyst. Besides, the confinement effect of TiNTs makes partial toxicants be trapped inside the tubular channel of TiNTs. So that protects the active components, which are distributed on the out wall of TiNTs, from being poisoned.

为了实现低温NH3-SCR技术的广泛应用,迫切需要一种具有高催化活性和较强低温抗中毒性能的环保型选择性催化还原(SCR)催化剂。选择合适的载体是提高SCR催化剂的催化活性和抗中毒能力的重要措施之一。采用浸渍法制备了传统二氧化钛(MnCe/TiO2)和钛酸盐纳米管(MnCe/TiNTs)负载的氧化锰-氧化铈,并在有或无SO2的烟气中评价了它们对NH3-SCR的催化活性;H2O。结果表明,将P25 TiO2在130℃下水热处理24 h,可以得到形貌和微观结构最优的TiNTs。在TiNTs上负载MnOx-CeO2复合材料不仅提高了低温催化活性,而且提高了N2选择性,拓宽了催化剂的活性温度窗。主要原因是TiNTs具有较大的比表面积和独特的空心管状结构,有利于催化活性组分在TiNTs的内外壁上高度分散,从而丰富了表面酸位和表面活性氧,实现低温SCR反应循环。此外,TiNTs显著提高了SO2 &催化剂的耐水性,减轻了SO2、H2O与反应物之间的竞争性吸附,使MnCe/TiNTs催化剂上的硫酸铵或硫酸氢铵的沉积更加困难。此外,TiNTs的约束效应使部分毒物被困在TiNTs的管状通道内。这样就可以保护分布在tint外壁的活性成分不受毒害。
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引用次数: 5
The Comparative Study of Reaction Mechanisms and Catalytic Performances of Cu–SSZ-13 and Fe–SSZ-13 for the NH3-SCR Reaction Cu-SSZ-13与Fe-SSZ-13对NH3-SCR反应机理及催化性能的比较研究
IF 3 4区 化学 Q3 CHEMISTRY, PHYSICAL Pub Date : 2022-02-28 DOI: 10.1007/s10563-022-09353-z
Kaiwei Qin, Lei Guo, Shujun Ming, Shoute Zhang, Yanbin Guo, Lei Pang, Tao Li

The catalytic performances and mechanism differences of model catalysts Cu–SSZ-13 and Fe–SSZ-13 with similar metal content and Si/Al ratio were compared. In the NH3-SCR reaction, Cu–SSZ-13 had a good NO conversion at low temperature, broad active temperature windows and better hydrothermal stability. Fe–SSZ-13 showed better high-temperature NO conversion rate and better resistance to sulfur poisoning, but poorer low-temperature NH3-SCR activity. NH3-TPD verified the content difference of L-NH3 and B-NH3 of Cu- and Fe–SSZ-13. UV–Vis DRS, EPR, H2-TPR indicated the active species of Cu- and Fe–SSZ-13. Results showed that Cu–SSZ-13 only had one type active species of Cu2+, Fe–SSZ-13 had Fe3+ species that acted as active centers at low temperature and reactivity oligomeric Fe species at high temperature. The diffuse reflection infrared Fourier transform spectrum (DRIFTS) results showed that the reactions of Cu–SSZ-13 and Fe–SSZ-13 at low temperature both followed the Eley–Rideal (E–R) mechanism and the Langmuir–Hinshelwood (L–H) mechanism. Cu–SSZ-13 could perform the catalytic process well under both mechanisms, but when Fe–SSZ-13 followed the E–R mechanism, there were many B-NH3 species, which was not conducive to the reaction. When following the L–H mechanism, the speed of NO3 participating in the reaction was slow due to ammonia inhibition, resulting in poor low-temperature activity.

比较了金属含量和硅铝比相近的Cu-SSZ-13和Fe-SSZ-13模型催化剂的催化性能和机理差异。在NH3-SCR反应中,Cu-SSZ-13具有较好的低温NO转化率、较宽的活性温度窗和较好的水热稳定性。Fe-SSZ-13具有较好的高温NO转化率和抗硫中毒能力,但低温NH3-SCR活性较差。NH3-TPD验证了Cu-和Fe-SSZ-13中L-NH3和B-NH3含量的差异。UV-Vis DRS、EPR、H2-TPR为Cu-和Fe-SSZ-13的活性物质。结果表明,Cu-SSZ-13只有一类Cu2+活性物质,Fe - ssz -13在低温下有Fe3+作为活性中心,在高温下有反应性低聚铁。漫反射红外傅里叶变换光谱(DRIFTS)结果表明,Cu-SSZ-13和Fe-SSZ-13在低温下的反应均遵循Eley-Rideal (E-R)机制和Langmuir-Hinshelwood (L-H)机制。Cu-SSZ-13在两种机制下都能很好地进行催化反应,而Fe-SSZ-13在E-R机制下存在较多的B-NH3,不利于反应的进行。当遵循L-H机制时,由于氨的抑制,NO3−参与反应的速度较慢,低温活性较差。
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引用次数: 6
期刊
Catalysis Surveys from Asia
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