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Technical failures in green hydrogen production and reliability engineering responses: Insights from database analysis and a literature review 绿色制氢过程中的技术故障和可靠性工程对策:数据库分析和文献综述的启示
IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-14 DOI: 10.1016/j.ijhydene.2024.11.129
Farhana Yasmine Tuhi , Marta Bucelli , Yiliu Liu
Green hydrogen represents a promising solution for renewable energy application and carbon footprint reduction. However, its production through renewable energy powered water electrolysis is hindered by significant cost, arising from repair, maintenance, and economic losses due to unexpected downtimes. Although reliability engineering is highly effective in addressing such issues, there is limited research on its application in the hydrogen field. To present the state-of-the-art research, this study aims to explore the potential of reducing these events through reliability engineering, a widely adopted approach in various industries. For this purpose, it examines past accidents occurred in water electrolysis plants from the hydrogen incident and accident database (HIAD 2.1). Besides, a literature review is performed to analyze the state-of-the-art application of reliability engineering techniques, such as failure analysis, reliability assessment, and reliability-centered maintenance, in the hydrogen sector and similar industries. The study highlights the contributions and potentials of reliability engineering for efficient and stable green hydrogen production, while also discussing the gaps in applying this approach. The unique challenges posed by hydrogen's physical properties and innovative technologies in water electrolysis plants necessitate advancement and specialized approaches for reliability engineering.
绿色氢气是可再生能源应用和减少碳足迹的一种有前途的解决方案。然而,通过以可再生能源为动力的水电解法生产氢气,却因维修、维护成本高昂以及意外停机造成的经济损失而受到阻碍。虽然可靠性工程在解决这些问题方面非常有效,但在氢能领域应用可靠性工程的研究却非常有限。为了介绍最新的研究成果,本研究旨在探索通过可靠性工程这一各行业广泛采用的方法来减少此类事件的可能性。为此,本研究从氢气事件和事故数据库 (HIAD 2.1) 中研究了过去在电解水厂发生的事故。此外,还进行了文献综述,分析了可靠性工程技术在氢能行业和类似行业中的最新应用,如故障分析、可靠性评估和以可靠性为中心的维护。研究强调了可靠性工程对高效稳定的绿色制氢的贡献和潜力,同时也讨论了应用这种方法的不足之处。氢的物理特性和水电解厂的创新技术带来了独特的挑战,因此有必要在可靠性工程方面采用先进和专业的方法。
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引用次数: 0
Electrocatalytic hydrogen evolution and in-situ observation of hydrogen microbubbles evolution on stainless steel meshes with various mesh numbers 电催化氢气进化以及原位观测不同网目数不锈钢网上氢气微气泡的进化情况
IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-14 DOI: 10.1016/j.ijhydene.2024.11.080
Shujuan Liu , Ruize Gu , Xiaomeng Diao , Dandan Liang , Weihua He
Stainless steel mesh (SSM) is a cost-effective, readily available catalyst and conductive substrate for large-scale hydrogen production in microbial electrolysis cells (MEC). This study reveals that variations in wire diameter and aperture size of SSM affect both the electroactive area for hydrogen evolution reaction (HER) and the formation and diffusion of hydrogen micro-nano bubbles, impacting MEC performance. In-situ hydrogen microbubble observation shows that 60-mesh SSM provides optimal hydrogen evolution due to its large electrochemical active area and many nucleation sites, minimizing the “bubble shielding effect”. The SSM-60 MEC achieves the highest hydrogen recovery (75 ± 5.1%) and energy recovery efficiency (85 ± 6.2%). This study combines electroactivity testing with microscopic in-situ reaction observation to provide a novel strategy for understanding efficient hydrogen evolution catalysts.
不锈钢网(SSM)是微生物电解池(MEC)中用于大规模制氢的一种具有成本效益、易于获得的催化剂和导电基质。本研究揭示了 SSM 的线径和孔径大小的变化会影响氢进化反应(HER)的电活性面积以及氢微纳气泡的形成和扩散,从而影响 MEC 的性能。原位氢气微气泡观测表明,60 目 SSM 具有较大的电化学活性面积和较多的成核点,最大程度地减少了 "气泡屏蔽效应",因此能提供最佳的氢气进化效果。SSM-60 MEC 实现了最高的氢回收率(75 ± 5.1%)和能量回收效率(85 ± 6.2%)。这项研究将电活性测试与微观原位反应观察相结合,为了解高效氢进化催化剂提供了一种新策略。
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引用次数: 0
Effect of oxygen enrichment and NH3 pre-cracking on laminar burning velocity and intrinsic instability of NH3/bio-syngas 富氧和 NH3 预裂解对 NH3/生物合成气层流燃烧速度和内在不稳定性的影响
IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-13 DOI: 10.1016/j.ijhydene.2024.11.121
Lijuan Wen, Qifeng Zhu, Jingwei Zeng, Haoxin Deng, Guoyan Chen, Xiaoping Wen, Fahui Wang, Qizheng Hao
This paper investigates the laminar burning velocity (SL) and instability of NH3/bio-syngas under different bio-syngas contents, oxygen enrichment factors (Ω), and the cracking ratio of NH3 (ζ) using a constant-volume combustion bomb. The results show that increasing bio-syngas, Ω, and ζ effectively enhance the SL of the fuel. Around ζ = 60%, the relationship between SL and the NH3 content before cracking is reversed. Increasing the bio-syngas and ζ enhance SL through the chemical effect, while Ω primarily enhances SL through the thermal effect. When Ω = 50%, the contribution of thermal effect can reach up to 94.53%. Linear stability analysis indicates that increasing the bio-syngas content and ζ reduces the critical Peclet number (Pec), while Ω increases Pec. As the bio-syngas content and ζ increase, the growth rate of perturbation () monotonically increases, indicating instability. Ω, on the other hand, decreases , making it negative.
本文使用恒容燃烧弹研究了不同生物合成气含量、富氧系数(Ω)和 NH3 裂解率(ζ)条件下 NH3/生物合成气的层燃速度(SL)和不稳定性。结果表明,增加生物合成气、Ω 和 ζ 能有效提高燃料的可燃性。在 ζ = 60% 左右,SL 与裂解前 NH3 含量之间的关系发生了逆转。增加生物合成气和 ζ 可通过化学效应提高 SL,而 Ω 则主要通过热效应提高 SL。当 Ω = 50% 时,热效应的贡献可达 94.53%。线性稳定性分析表明,增加生物合成气含量和 ζ 会降低临界佩克莱特数(Pec),而 Ω 会增加临界佩克莱特数。随着生物合成气含量和 ζ 的增加,扰动增长率(∑)单调增加,表明不稳定。而 Ω 则会降低 ∑,使其成为负值。
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引用次数: 0
Application and performance Enhancement of acetic acid-Regulated ligand defect engineering in NiMOF electrocatalysts 醋酸调节配体缺陷工程在 NiMOF 电催化剂中的应用和性能提升
IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-13 DOI: 10.1016/j.ijhydene.2024.10.366
Nana Wang , Sunpeng Shan , Lijun Huang, Xiao Zhang, Zhiwei Shu, Qiang Zhang, Yanchao Xu, Jianrong Chen, Yang Jiao
Introducing organic ligands into metal-organic frameworks (MOFs) is an effective method for preparing defective MOFs. This approach enables the fabrication of cost-effective, efficient, highly conductive, and richly active-site electrocatalysts. Herein, the defective NiMOF is synthesized via a straightforward one-pot solvothermal method by partially substituting phthalic acid (PTA) ligands with acetic acid (HOAc), which effectively regulates the micro-morphology and electronic structure of the NiMOF nanoflowers, thus creating abundant electrochemical active sites, significantly improving electronic conductivity and promoting rapid charge transfer. The resulting DE-NiMOF-0.5 nanoflowers, prepared with HOAc substitution, demonstrate excellent electrochemical performance at a current density of 10 mA cm−2, the hydrogen evolution reaction (HER) overpotential is 188 mV (Tafel slope of 175 mV dec−1), while the oxygen evolution reaction (OER) overpotential is 205 mV (Tafel slope of 37 mV dec−1). The introduction of acetic acid ligands in DE-NiMOF-0.5 not only constructs the ligand defects within the catalyst, but also increases the abundant active sites, enhancing the hydrophilicity of the catalyst and facilitating electronic transfer between the catalyst surface and the electrolyte. This study explores a strategy for preparing defective MOF catalysts through introducing modulators, providing an economically viable material pathway for electrocatalysis and opening new possibilities for designing and synthesizing efficient electrocatalysts in future research endeavors.
将有机配体引入金属有机框架(MOFs)是制备缺陷 MOFs 的有效方法。通过这种方法可以制备出具有成本效益、高效、高导电性和丰富活性位的电催化剂。本文通过乙酸(HOAc)部分取代邻苯二甲酸(PTA)配体,采用简单的一锅溶热法合成了缺陷NiMOF,有效地调节了NiMOF纳米花的微观形貌和电子结构,从而形成了丰富的电化学活性位点,显著提高了电子传导性,促进了电荷的快速转移。用 HOAc 取代制备的 DE-NiMOF-0.5 纳米花束在 10 mA cm-2 的电流密度下表现出优异的电化学性能,氢进化反应(HER)过电位为 188 mV(Tafel 斜坡为 175 mV dec-1),而氧进化反应(OER)过电位为 205 mV(Tafel 斜坡为 37 mV dec-1)。在 DE-NiMOF-0.5 中引入醋酸配体不仅能在催化剂内部构建配体缺陷,还能增加丰富的活性位点,增强催化剂的亲水性,促进催化剂表面与电解质之间的电子转移。本研究探索了一种通过引入调制剂制备缺陷 MOF 催化剂的策略,为电催化提供了一种经济可行的材料途径,并为未来研究工作中设计和合成高效电催化剂提供了新的可能性。
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引用次数: 0
Soot formation in laminar ammonia-ethylene counterflow diffusion flames: Isolation of chemical, thermal, and dilution effects 层流氨-乙烯逆流扩散火焰中烟尘的形成:化学效应、热效应和稀释效应的分离
IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-13 DOI: 10.1016/j.ijhydene.2024.11.137
Zhicong Li , Shijia Liu , Chun Lou , Nimeti Kalaycı , Zhongnong Zhang , Kai Zhao , Songzhen Tang
This numerical study investigates the effect of ammonia (NH3) addition on soot formation in laminar ethylene counterflow diffusion flames (CDFs). A chemically inert species is used to isolate the chemical effect, while the thermal and dilution effects are isolated using the formation rate fitting method. The KM2-NH3 mechanism is constructed, demonstrating good applicability for modeling NH3–C2H4 CDFs. As the NH3 addition ratio (XNH3) increases, the peak temperature, benzene (A1) mole fraction, and soot volume fraction (SVF) decrease. The chemical effect of NH3 addition promotes temperature though R1: H + O2O + OH and R1927: NH2 + NHN2H2 + H. It also promotes A1 formation by boosting R298: 2C2H3 → A1, etc., and converts C4H6-13 to produce C3H3. However, it suppresses soot formation through surface growth SR42: open (se) + C2H2 → H (se) + 2C(B) + H. The dilution effect on suppressing A1 formation is stronger than the thermal effect. The thermal effect dominates the suppression of soot formation, and the chemical effect is stronger than the dilution effect at low XNH3, while the opposite is true at high XNH3.
本数值研究探讨了添加氨气(NH3)对层流乙烯逆流扩散火焰(CDF)中烟尘形成的影响。使用化学惰性物质隔离化学效应,同时使用形成率拟合方法隔离热效应和稀释效应。构建的 KM2-NH3 机理证明了 NH3-C2H4 CDF 建模的良好适用性。随着 NH3 添加比(XNH3)的增加,峰值温度、苯(A1)摩尔分数和烟尘体积分数(SVF)都会降低。添加 NH3 的化学效应通过 R1:H + O2O + OH 和 R1927 升温:它还通过提高 R298:2C2H3 → A1 等促进 A1 的形成,并将 C4H6-13 转化为 C3H3。然而,它通过表面生长 SR42 抑制烟尘的形成:open (se) + C2H2 → H (se) + 2C(B) + H。在低 XNH3 条件下,热效应在抑制烟尘形成方面占主导地位,化学效应强于稀释效应,而在高 XNH3 条件下则相反。
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引用次数: 0
Maximizing methane and hydrogen delivery capacity by carbon and boron nitride nanoscrolls 利用碳和氮化硼纳米卷轴最大限度地提高甲烷和氢气输送能力
IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-13 DOI: 10.1016/j.ijhydene.2024.11.138
Xuan Peng
The CH4 and H2 delivery capacity of carbon and boron nitride (BN) nanoscrolls was investigated, with a focus on optimizing the interlayer and van der Waals spacings to meet the U.S. Department of Energy (DOE) targets. Through computational simulations, the effects of interlayer spacing on CH4 and H2 adsorption were evaluated, revealing that while delivery quantities increase with interlayer spacing, achieving DOE targets remains a challenge for CH4. Notably, BN nanoscrolls exhibited higher adsorption capacities compared to carbon nanoscrolls, especially under low-pressure conditions. Conversely, carbon nanoscrolls displayed greater release quantities than BN nanoscrolls. For H2, delivery quantities met DOE targets at larger interlayer spacings, with carbon nanoscrolls requiring a spacing greater than 0.9 nm and BN nanoscrolls greater than 1.1 nm. For CH4 delivery, temperature optimization showed significant peaks in delivery for carbon nanoscrolls at 248 K. In contrast, BN nanoscrolls did not exhibit a peak in delivery. In carbon nanoscrolls, the optimal weight and volumetric capacities for methane delivery are 0.275 g/g and 182 cm3/cm3, respectively. Meanwhile, for hydrogen, the maximum delivery achieved is 8.26 wt% and 0.044 kg/L, which surpasses the DOE's storage target of 5.5 wt% and 0.04 kg/L. The study also highlighted the importance of structural parameter optimization, with a significant increase in weight delivery (>500%) and in volume delivery (>120%) for both gases.
研究了碳和氮化硼(BN)纳米卷轴的 CH4 和 H2 输送能力,重点是优化层间和范德华间距,以达到美国能源部(DOE)的目标。通过计算模拟,评估了层间间距对 CH4 和 H2 吸附的影响,结果表明,虽然输送量随层间间距的增加而增加,但实现 DOE 目标对 CH4 来说仍然是一个挑战。值得注意的是,与碳纳米卷轴相比,BN 纳米卷轴表现出更高的吸附能力,尤其是在低压条件下。相反,碳纳米卷比 BN 纳米卷的释放量更大。对于 H2,当层间间距较大时,释放量可达到 DOE 目标,碳纳米卷需要大于 0.9 nm 的间距,而 BN 纳米卷需要大于 1.1 nm 的间距。对于 CH4 的输送,温度优化显示碳纳米卷在 248 K 时的输送量达到显著峰值。碳纳米卷轴输送甲烷的最佳重量和体积容量分别为 0.275 g/g 和 182 cm3/cm3。同时,氢气的最大输送量为 8.26 wt% 和 0.044 kg/L,超过了能源部设定的 5.5 wt% 和 0.04 kg/L 的储存目标。研究还强调了结构参数优化的重要性,两种气体的重量输送量(500%)和体积输送量(120%)都有显著提高。
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引用次数: 0
Experimental and simulated study of ammonia blending with DME steam reformed and cracked gases under lean-burn condition 贫燃条件下合成氨与二甲醚蒸汽转化气和裂解气混合的实验和模拟研究
IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-13 DOI: 10.1016/j.ijhydene.2024.10.177
Xuanrui Zhang , Xiangyu Meng , Wenchao Zhu , Wuqiang Long , Mingshu Bi
Dimethyl ether (DME) steam reforming (SR) and cracking (CR) can not only achieve on-line production of hydrogen (H2) and methane (CH4) but also increase fuel energy. The ammonia blending with DME-SR or DME-CR gases is an effective method to enhance the reactivity of ammonia combustion. This paper aims to compare the effects of DME-SR and DME-CR on combustion and emissions under lean-burn condition. In the constant volume combustion chamber (CVCC) experiments, the in-chamber pressure and flame propagation process were measured for NH3/H2 and NH3/CH4 blends, and NO emissions were visualized by chemiluminescence. A three-dimensional (3D) model was established with validation by the experimental data. Based on this model, the effects of DME-SR and DME-CR on combustion process and NOx emissions were studied. The results showed that both DME-SR and DME-CR can enhance the ammonia combustion process under lean-burn condition. The case with DME energy ratio 70% and the equivalence ratio of 0.4 for SR (X70ER0.4-SR), and X30ER0.5-SR can achieve faster combustion rates than pure ammonia at ER of 1.0 (X0ER0.9) due to the main reforming product of H2. The ammonia blended with fuels from DME-SR and CR can help to improve the NO emission under lean-burn condition, being lower than X0ER0.9. These findings highlight the advantages of using DME-SR and DME-CR for improving the ammonia combustion. Considering the fuel energy increment, DME-CR could be potential to obtain better fuel economy and emission improvement in real engine application.
二甲醚(DME)蒸汽重整(SR)和裂解(CR)不仅能实现氢气(H2)和甲烷(CH4)的在线生产,还能增加燃料能量。氨与二甲醚-SR 或二甲醚-CR 气体混合是提高氨燃烧反应性的有效方法。本文旨在比较 DME-SR 和 DME-CR 在贫燃条件下对燃烧和排放的影响。在恒容燃烧室(CVCC)实验中,测量了 NH3/H2 和 NH3/CH4 混合物的腔内压力和火焰传播过程,并用化学发光法观察了氮氧化物的排放。通过实验数据的验证,建立了一个三维(3D)模型。基于该模型,研究了 DME-SR 和 DME-CR 对燃烧过程和氮氧化物排放的影响。结果表明,在贫燃烧条件下,DME-SR 和 DME-CR 都能增强氨的燃烧过程。二甲醚能量比为 70%、SR 的等效比为 0.4(X70ER0.4-SR)和 X30ER0.5-SR 的情况下,由于主要重整产物为 H2,其燃烧速率比 ER 为 1.0(X0ER0.9)的纯氨更快。与二甲醚-SR 和 CR 燃料混合的氨有助于改善贫燃条件下的氮氧化物排放,低于 X0ER0.9。这些发现凸显了使用 DME-SR 和 DME-CR 改善氨燃烧的优势。考虑到燃料能量的增加,DME-CR 有可能在实际发动机应用中获得更好的燃油经济性和排放改善。
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引用次数: 0
A deep learning method based on CNN-BiGRU and attention mechanism for proton exchange membrane fuel cell performance degradation prediction 基于 CNN-BiGRU 和注意机制的质子交换膜燃料电池性能退化预测深度学习方法
IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-13 DOI: 10.1016/j.ijhydene.2024.11.127
Jiaming Zhou , Xing Shu , Jinming Zhang , Fengyan Yi , Chunchun Jia , Caizhi Zhang , Xianghao Kong , Junling Zhang , Guangping Wu
The performance of proton exchange membrane fuel cells (PEMFCs) will gradually deteriorate during long-term operation. Accurate performance degradation prediction is crucial for extending the lifespan and improve the durability of fuel cells. This paper proposes a deep learning method (CNN-BiGRU-AM) that incorporates convolutional neural network (CNN), bidirectional gated recurrent unit (BiGRU) and attention mechanism (AM) for fuel cell degradation prediction. In the proposed method, CNN extracts complex features from the input data through convolutional operations, BiGRU models temporal information by considering both forward and reverse directions of the input sequence, and attention mechanism highlights key information in the input data through weight allocation. The proposed method is validated using long-term experimental data from fuel cells under steady-state and quasi-dynamic conditions. The results indicate that the absolute error of the proposed method is less than 1.2 mV for 97.94% of the data samples under steady-state conditions and less than 1.2 mV for 94.82% of the data samples under quasi-dynamic conditions. The prediction accuracy and stability of the proposed method are significantly improved compared to other deep learning prediction methods.
质子交换膜燃料电池(PEMFC)在长期运行过程中性能会逐渐退化。准确的性能退化预测对于延长燃料电池的使用寿命和提高其耐用性至关重要。本文提出了一种深度学习方法(CNN-BiGRU-AM),该方法结合了卷积神经网络(CNN)、双向门控递归单元(BiGRU)和注意力机制(AM),用于燃料电池退化预测。在所提出的方法中,卷积神经网络通过卷积运算从输入数据中提取复杂特征,双向门控递归单元通过考虑输入序列的正向和反向来建立时间信息模型,而注意力机制则通过权重分配来突出输入数据中的关键信息。利用燃料电池在稳态和准动态条件下的长期实验数据对所提出的方法进行了验证。结果表明,在稳态条件下,97.94% 的数据样本的绝对误差小于 1.2 mV;在准动态条件下,94.82% 的数据样本的绝对误差小于 1.2 mV。与其他深度学习预测方法相比,拟议方法的预测精度和稳定性都有显著提高。
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引用次数: 0
Numerical study of the spontaneous ignition mechanisms of pressurized hydrogen released inside pipes with different structures 对不同结构管道内释放的加压氢气自燃机制的数值研究
IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-13 DOI: 10.1016/j.ijhydene.2024.11.117
Haowei Qiu , Rui Zhou , Xing Li , Jun Li , Hongyu Huang
Hydrogen is considered a key clean energy carrier to achieve the global goal of carbon neutrality. But spontaneous ignition can occur when pressurized hydrogen is released into pipes, and the presence of different pipe structures will significantly affect the ignition mechanism. In this work, the effects of varied pipe structures on the shock wave propagation and spontaneous ignition characteristics are investigated by numerical simulation with the DNS-like approach, EDC combustion model, and 21-step detailed hydrogen combustion mechanism. Results show that the simulation is in well agreement with the experimental data. Five dominant spontaneous ignition mechanisms are provided depending on different pipe structures. Among all types of pipe structures investigated, contraction structures can lead to a greater increase in shock wave pressure due to more severe shock wave reflection and convergence. While enlargement structures can contribute to more mixing of hydrogen and air, causing more sufficient combustion. This study provides a comprehensive understanding and clear safety guidance to inform the practical application of hydrogen energy.
氢气被认为是实现全球碳中和目标的关键清洁能源载体。但是,当加压氢气被释放到管道中时可能会发生自燃,而不同管道结构的存在会对点火机制产生重大影响。本研究采用类 DNS 方法、EDC 燃烧模型和 21 步详细氢气燃烧机理,通过数值模拟研究了不同管道结构对冲击波传播和自燃特性的影响。结果表明,模拟结果与实验数据十分吻合。根据不同的管道结构,提供了五种主要的自燃机制。在所有被研究的管道结构类型中,收缩结构会由于更严重的冲击波反射和汇聚而导致冲击波压力的更大增加。而扩大型结构则会促进氢气和空气的混合,从而引起更充分的燃烧。这项研究为氢能的实际应用提供了全面的认识和明确的安全指导。
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引用次数: 0
Effect of support morphology on the ammonia synthesis activity of Ru/CeO2-based catalysts 支撑体形态对基于 Ru/CeO2 催化剂的氨合成活性的影响
IF 8.1 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2024-11-13 DOI: 10.1016/j.ijhydene.2024.11.053
Kiyoshi Yamazaki , Yoshihiro Goto , Masashi Kikugawa , Akinori Sato , Yuichi Manaka , Tetsuya Nanba , Hideyuki Matsumoto , Shinichi Ookawara
We investigate the effect of the support morphology on ammonia (NH3) synthesis activity of Ru/CeO2-based catalysts using supports derived from various CeO2 materials under different treatment temperatures with different SiO2/ZrO2 additions. These supports are classified by peak pore size into three pore structure types: small (3–4 nm), medium (7–20 nm), and large (50–70 nm). The medium-type supports show the highest specific surface area (SSA), which increases with SiO2/ZrO2 addition. The Ru dispersion on each support, regardless of its type and composition, is determined from its SSA. The NH3-synthesis activity of catalysts at 0.1 MPa and a space velocity (SV) of 36000 h−1 exhibits a volcanic trend with respect to the Ru dispersion. This is explained by the fraction of active B5-type sites generated. At SVs >72000 h−1, the activity of catalysts with peak pore size <8 nm is less than the above volcanic trend, possibly owing to increased diffusion resistance in the pore.
我们研究了支撑体形态对 Ru/CeO2 基催化剂合成氨 (NH3) 活性的影响,使用的支撑体来自不同处理温度下添加不同 SiO2/ZrO2 的各种 CeO2 材料。这些载体按峰值孔径分为三种孔结构类型:小型(3-4 nm)、中型(7-20 nm)和大型(50-70 nm)。中型支撑物的比表面积(SSA)最大,随着 SiO2/ZrO2 添加量的增加而增大。无论支撑物的类型和组成如何,Ru 在每种支撑物上的分散度都是根据其 SSA 确定的。在 0.1 MPa 和 36000 h-1 的空间速度 (SV) 条件下,催化剂的 NH3 合成活性与 Ru 的分散度有关,呈现出火山爆发的趋势。这可以从生成的活性 B5 型位点的比例得到解释。在 SVs >72000 h-1 条件下,峰值孔径为 8 nm 的催化剂的活性低于上述火山岩趋势,这可能是由于孔中的扩散阻力增加所致。
{"title":"Effect of support morphology on the ammonia synthesis activity of Ru/CeO2-based catalysts","authors":"Kiyoshi Yamazaki ,&nbsp;Yoshihiro Goto ,&nbsp;Masashi Kikugawa ,&nbsp;Akinori Sato ,&nbsp;Yuichi Manaka ,&nbsp;Tetsuya Nanba ,&nbsp;Hideyuki Matsumoto ,&nbsp;Shinichi Ookawara","doi":"10.1016/j.ijhydene.2024.11.053","DOIUrl":"10.1016/j.ijhydene.2024.11.053","url":null,"abstract":"<div><div>We investigate the effect of the support morphology on ammonia (NH<sub>3</sub>) synthesis activity of Ru/CeO<sub>2</sub>-based catalysts using supports derived from various CeO<sub>2</sub> materials under different treatment temperatures with different SiO<sub>2</sub>/ZrO<sub>2</sub> additions. These supports are classified by peak pore size into three pore structure types: small (3–4 nm), medium (7–20 nm), and large (50–70 nm). The medium-type supports show the highest specific surface area (SSA), which increases with SiO<sub>2</sub>/ZrO<sub>2</sub> addition. The Ru dispersion on each support, regardless of its type and composition, is determined from its SSA. The NH<sub>3</sub>-synthesis activity of catalysts at 0.1 MPa and a space velocity (SV) of 36000 h<sup>−1</sup> exhibits a volcanic trend with respect to the Ru dispersion. This is explained by the fraction of active B<sub>5</sub>-type sites generated. At SVs &gt;72000 h<sup>−1</sup>, the activity of catalysts with peak pore size &lt;8 nm is less than the above volcanic trend, possibly owing to increased diffusion resistance in the pore.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"94 ","pages":"Pages 406-419"},"PeriodicalIF":8.1,"publicationDate":"2024-11-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142657012","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
期刊
International Journal of Hydrogen Energy
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