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International Journal of Hydrogen Energy最新文献

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In-situ synthesis of hexagonal SnS2 on 2D layered Ti3C2Tx/g-C3N4 nano-heterostructures for enhanced photocatalytic H2 generation via water splitting and HER applications 在二维层状Ti3C2Tx/g-C3N4纳米异质结构上原位合成六方SnS2以增强水裂解光催化制氢和HER应用
IF 9.2 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-07-22 Epub Date: 2026-06-28 DOI: 10.1016/j.ijhydene.2026.156241
Amol B. Tambe, Satish K. Pardeshi
The successful in-situ hydrothermal synthesis of 2D Ti3C2Tx/g-C3N4/SnS2 nano-heterostructures with different Ti3C2Tx:g-C3N4 ratios is demonstrated in this work. These structures were then assessed as photocatalytic for hydrogen production using water splitting and hydrogen evolution studies. To verify the creation and characteristics of the nano-heterostructures, a number of characterisation techniques were used. The XRD examination confirmed the effective synthesis of Ti3C2Tx/g-C3N4/SnS2 nano-heterostructures by revealing diffraction peaks corresponding to Ti3C2Tx, g-C3N4, and SnS2. The creation of 2D nano-heterostructures was further confirmed by the FE-SEM, HR-TEM, and XPS, which revealed layered structures of MXene, hexagonal nanosheets of SnS2, and nanosheets of g-C3N4. The coexistence of Ti3C2Tx, g-C3N4, and SnS2 in the nano-heterostructures was revealed by the high-resolution TEM images and selected area electron diffraction (SAED) patterns. With band gaps ranging from 2.11 to 2.70 eV, the optical characteristics of the nano-heterostructures demonstrated absorption in the visible light spectrum. With the exception g-C3N4, all compositions showed band-edge emission in the 471-495 nm range in the photoluminescence (PL) spectra. Significantly exceeding other compositions, the TSC-75% nano-heterostructure showed the highest photocatalytic hydrogen generation of about 2960.4 μmol/0.1g along with an outstanding apparent quantum yield of 4.8%. The TSC-75% has a low overpotential value of 92.2 mV and an excellent Tafel slope of 109.7 mV.dec−1 in a 1 M KOH electrolyte at a current density of −10 mA cm−2.The electrochemical double layer capacitance of TSC-75% (14.12 mFcm−2) was found to be 3.9 times higher than Ti3C2Tx (3.57 mFcm−2), 13.8 times higher than g-C3N4 (1.02 mFcm−2), and 1.5 times higher than SnS2 (9.41 mFcm−2). The potential for HER reduction is increased by the in-situ growing SnS2 nanoplates because they enhance hydrogen adsorption active sites, promote charge transfer, and help establish electrochemical stability up to 30 h. Electrochemical impedance spectroscopy, steady state PL spectroscopy, and time resolved PL decay kinetics all validate the successful electron transport mechanism at the TSC-75% interface. These results imply that photocatalytic effectiveness can be greatly increased by designing 2D nano-heterostructures with optimum composition.
本文成功地原位水热合成了具有不同Ti3C2Tx:g-C3N4比例的二维Ti3C2Tx/g-C3N4/SnS2纳米异质结构。然后利用水裂解和析氢研究评估了这些结构的光催化产氢能力。为了验证纳米异质结构的产生和特性,使用了许多表征技术。XRD检测显示Ti3C2Tx、g-C3N4和SnS2对应的衍射峰,证实了Ti3C2Tx/g-C3N4/SnS2纳米异质结构的有效合成。通过FE-SEM, HR-TEM和XPS进一步证实了二维纳米异质结构的形成,揭示了MXene的层状结构,SnS2的六边形纳米片和g-C3N4的纳米片。通过高分辨率TEM图像和选择区域电子衍射(SAED)图揭示了Ti3C2Tx、g-C3N4和SnS2在纳米异质结构中的共存。带隙在2.11 ~ 2.70 eV范围内,纳米异质结构的光学特性表现为可见光吸收。除g-C3N4外,其余化合物均在471 ~ 495 nm范围内发光。TSC-75%纳米异质结构的光催化产氢量最高,约为2960.4 μmol/0.1g,表观量子产率为4.8%。TSC-75%在1 M KOH电解液中,电流密度为- 10 mA cm−2时,过电位值为92.2 mV, Tafel斜率为109.7 mV.dec−1。TSC-75%的电化学双层电容(14.12 mFcm−2)比Ti3C2Tx (3.57 mFcm−2)高3.9倍,比g-C3N4 (1.02 mFcm−2)高13.8倍,比SnS2 (9.41 mFcm−2)高1.5倍。原位生长SnS2纳米板增加了氢吸附活性位点,促进了电荷转移,并有助于建立高达30 h的电化学稳定性,从而增加了HER还原的潜力。电化学阻抗谱、稳态PL谱和时间分辨PL衰减动力学都验证了TSC-75%界面上成功的电子传递机制。这些结果表明,设计具有最佳组成的二维纳米异质结构可以大大提高光催化效率。
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引用次数: 0
Construction of all-solid-state Z-scheme CdZnS/CNT/CuCo2S4 heterojunction for enhanced photocatalytic hydrogen production and tetracycline degradation 全固态Z-scheme CdZnS/CNT/CuCo2S4异质结的构建促进光催化制氢和四环素降解
IF 9.2 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-07-22 Epub Date: 2026-06-28 DOI: 10.1016/j.ijhydene.2026.156213
Yuqi Wang, Yu Li, Kaige Huang, Mengmeng Ma, Zhanwei Shen, Aiwei Tang, Xiaomin Dou, Shizhong Yue, Zhijie Wang
Simultaneous achievement of green hydrogen production and pollutant removal is an attractive approach for mitigating energy scarcity and environmental pollution. This work successfully constructed an all-solid-state CdZnS/CNT/CuCo2S4 Z-scheme heterojunction via a combined hydrothermal and solvent evaporation approach, enabling highly efficient bifunctional photocatalytic performance in hydrogen production and tetracycline removal. Benefiting from visible light excitation, the tailored CdZnS/CNT/CuCo2S4 heterostructure delivered an outstanding photocatalytic H2 generation activity, as high as 10.29 mmol g−1 h−1. The catalytic performance was 3.3 times superior to pristine CdZnS. Moreover, it achieved 92.3% degradation of tetracycline within 30 min. The boosted photocatalytic performance originates from the Z-type charge transmission pathway supported by CNT electron bridges, significantly promoting carrier separation and transport. Excited electrons in CdZnS reduce water to produce hydrogen, while the holes in CuCo2S4 degrade tetracycline. This study paves a rational pathway for the fabrication of Z-scheme heterojunction photocatalysts that employ carbon nanotubes as electron mediators.
同时实现绿色制氢和污染物去除是缓解能源短缺和环境污染的一个有吸引力的途径。本工作通过水热和溶剂蒸发相结合的方法成功构建了全固态CdZnS/CNT/CuCo2S4 Z-scheme异质结,实现了高效的双功能光催化产氢和去除四环素的性能。得益于可见光激发,定制的CdZnS/CNT/CuCo2S4异质结构具有出色的光催化H2生成活性,高达10.29 mmol g−1 h−1。催化性能是原始CdZnS的3.3倍。在30 min内对四环素的降解达到92.3%。提高的光催化性能源于碳纳米管电子桥支持的z型电荷传输路径,显著促进载流子分离和输运。CdZnS中的激发态电子还原水生成氢,而CuCo2S4中的空穴降解四环素。本研究为制备以碳纳米管为电子介质的z型异质结光催化剂开辟了一条合理的途径。
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引用次数: 0
Probabilistic techno-economic analysis of blue hydrogen production under natural gas price and capital cost index uncertainty 天然气价格和资本成本指数不确定性下蓝色制氢的概率技术经济分析
IF 9.2 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-07-22 Epub Date: 2026-06-27 DOI: 10.1016/j.ijhydene.2026.156268
Dong Guk Kim, Yoo Ri Kim, Dong Hwi Jeong
Blue hydrogen is attracting attention as a practical low-carbon pathway, but its economic viability remains uncertain, especially in small-scale processes where feedstock and equipment costs strongly affect performance. The long-term economic effects of time-varying external variables have not been fully explored. Here, using Aspen Plus simulation, time-series forecasting, and Monte Carlo simulation, we develop a probabilistic techno-economic framework that incorporates natural gas price and the chemical engineering plant cost index (CEPCI). The natural gas price was modeled using a mean-reverting autoregressive model, and the CEPCI using a break-point autoregressive model. These forecasts were integrated with process simulation results to estimate levelized cost of hydrogen distributions and screen operating conditions using P50, P95, and conditional value at risk (CVaR). The framework enables operating conditions to be evaluated based on both expected cost performance and upper-tail cost risk under uncertain future market conditions.
蓝氢作为一种实用的低碳途径正引起人们的关注,但其经济可行性仍不确定,特别是在原料和设备成本严重影响性能的小规模工艺中。时变外部变量的长期经济影响尚未得到充分探讨。在这里,我们使用Aspen Plus模拟、时间序列预测和蒙特卡罗模拟,开发了一个包含天然气价格和化工工厂成本指数(CEPCI)的概率技术经济框架。天然气价格采用均值回归自回归模型,CEPCI采用断点自回归模型。这些预测与过程模拟结果相结合,利用P50、P95和条件风险值(CVaR)来估计氢气分布的平准化成本和筛选操作条件。该框架能够在不确定的未来市场条件下,根据预期成本绩效和上尾成本风险对运营状况进行评估。
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引用次数: 0
Optimizing demand-side management in smart grid with renewable energy sources using SBOA-QCGNN approach 基于SBOA-QCGNN方法的可再生能源智能电网需求侧管理优化
IF 9.2 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-07-22 Epub Date: 2026-06-26 DOI: 10.1016/j.ijhydene.2026.155737
Haewon Byeon, M.S.Sivagama Sundari
Smart grids have transformed current energy markets, allowing users to participate in demand response programs, yet users struggle due to low awareness. The proposed approach combines the SBOA and QCGNN, which is termed the SBOA-QCGNN technique. The primary goals of the proposed approach are to lower carbon emissions, lower power bill costs, and lessen load profile variation. The SBOA is utilized to optimize consumers' energy consumption, while QCGNN is used to predict electricity produced by RES. The proposed technique is evaluated and compared to existing techniques using the MATLAB platform. The proposed technique determines superior results compared to existing methods like PSO, GWO, and GA. The proposed strategy achieves a cost of 10$, a 10.5% reduction in carbon emissions, a PAR of 3.04, and a computation time of 1.41 s, showing better performance than existing methods. This approach offers a solution improving economic and environmental sustainability, enabling efficient energy management.
智能电网已经改变了当前的能源市场,允许用户参与需求响应计划,但用户由于意识不足而挣扎。该方法将SBOA和QCGNN相结合,称为SBOA-QCGNN技术。提出的方法的主要目标是降低碳排放,降低电费成本,并减少负荷分布的变化。利用SBOA来优化消费者的能源消耗,而QCGNN用于预测res产生的电力。利用MATLAB平台对所提出的技术进行了评估并与现有技术进行了比较。与现有的PSO、GWO和GA等方法相比,该技术具有更好的效果。该策略的成本为10美元,碳排放量减少10.5%,PAR为3.04,计算时间为1.41 s,性能优于现有方法。这种方法提供了一种改善经济和环境可持续性的解决方案,实现了高效的能源管理。
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引用次数: 0
Experimental and numerical study on the explosion characteristics of CO/H2 mixtures with trace Cl2 and HCl addition 添加微量Cl2和HCl的CO/H2混合物爆炸特性的实验和数值研究
IF 9.2 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-07-22 Epub Date: 2026-06-28 DOI: 10.1016/j.ijhydene.2026.156232
Xing Liu, Quanbin Ren, Yuanqi Bai, Yitong Wang
This study investigated the effects of N2-diluted Cl2 and HCl on the explosion characteristics and lower flammability limit (LFL) of CO/H2 mixtures through experiments and numerical simulations. The experimental results indicated that under fuel-rich conditions, the HCl group exhibited a stronger inhibitory effect on combustion than the Cl2 group, whereas the opposite was true under fuel-lean and high chlorine loading conditions. Both Cl2 and HCl significantly increased the lower flammability limit of the syngas, and the extent of this increase was comparable. Kinetic analysis and CFD simulations revealed that Cl2 promoted early ignition and exacerbated cellular instability in the flame front, yet was constrained by thermodynamic limitations at low equivalence ratios; in contrast, the early-promoting effect of HCl was negligible, and its chemical suppression effect remained dominant throughout. Furthermore, a sensitivity analysis of the laminar flame speed at the LFL was conducted to identify the key suppression reactions.
通过实验和数值模拟研究了n2稀释Cl2和HCl对CO/H2混合物爆炸特性和燃烧下限的影响。实验结果表明,在富燃料条件下,HCl组对燃烧的抑制作用强于Cl2组,而在低燃料和高氯负荷条件下则相反。Cl2和HCl均显著提高了合成气的可燃性下限,且这种提高的程度具有可比性。动力学分析和CFD模拟表明,Cl2促进了早期点火,加剧了火焰前的细胞不稳定性,但在低当量比时受到热力学限制;相比之下,HCl的早期促进作用可以忽略不计,其化学抑制作用始终占主导地位。此外,本文还对低燃烧层的层流火焰速度进行了灵敏度分析,以确定关键的抑制反应。
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引用次数: 0
Comprehensive analysis of on-sun catalytic reforming of methane with a hydroxyapatite-supported nickel catalyst in a tubular solar reactor 管式太阳能反应器中羟基磷灰石负载镍催化剂催化重整甲烷的综合分析
IF 9.2 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-07-22 Epub Date: 2026-06-28 DOI: 10.1016/j.ijhydene.2026.156212
Srirat Chuayboon, Ratikorn Kulporm, Sompong O-Thong, Doan Pham Minh, Stéphane Abanades
Methane reforming offers a suitable pathway for greenhouse gas utilization, but its implementation is hindered by catalyst deactivation due to carbon deposition and thermal sintering. This study shows that hydroxyapatite serves as a stable catalytic support for solar-driven dry, steam, and dual reforming. The influence of oxidizer type and concentration (H2O, CO2, H2O/CO2 mixture) is experimentally investigated at 800 °C in a tubular solar reactor. A hydroxyapatite-supported nickel catalyst (Ni/HA) achieves methane conversion exceeding 95% with 95% H2 and 96% CO selectivity. An excess of oxidant (oxidant/CH4 mole ratio of 1.2-1.5) is recommended to promote CH4 conversion, improve solar reactor performance, and prevent carbon formation and catalyst deactivation. Through sequential on-sun experimental runs, energy upgrade factor above 1.5 and solar-to-fuel efficiency over 20% are attained, demonstrating high catalytic performance stabilized by the metal dispersion on the support. Dual reforming exhibits the highest syngas yield and performance, with minimized carbon formation and H2/CO ratio approaching 2.0. Catalyst characterization (XRD, FTIR, SEM, TEM/EDX) confirms high thermal/chemical stability of Ni/HA under solar heating conditions. These results demonstrate compatibility of Ni/HA catalyst with solar methane reforming, providing a high-efficiency sustainable system for converting greenhouse gases into syngas.
甲烷重整为温室气体的利用提供了一条合适的途径,但由于碳沉积和热烧结导致催化剂失活,阻碍了甲烷重整的实施。该研究表明,羟基磷灰石作为一种稳定的催化载体,可用于太阳能驱动的干式、蒸汽式和双重重整。在800 °C的管式太阳能反应器中,实验研究了氧化剂类型和浓度(H2O、CO2、H2O/CO2混合物)的影响。羟基磷灰石负载镍催化剂(Ni/HA)的甲烷转化率超过95%,H2选择性为95%,CO选择性为96%。过量的氧化剂(氧化剂/CH4摩尔比为1.2-1.5)可以促进CH4的转化,提高太阳能反应器的性能,防止碳的形成和催化剂的失活。通过连续的太阳实验运行,能量升级系数超过1.5,太阳能-燃料效率超过20%,显示出高催化性能稳定的金属分散在支架上。双重整具有最高的合成气产率和性能,生成碳最少,H2/CO比接近2.0。催化剂表征(XRD, FTIR, SEM, TEM/EDX)证实了Ni/HA在太阳能加热条件下具有很高的热/化学稳定性。这些结果证明了Ni/HA催化剂与太阳能甲烷重整的相容性,为温室气体转化为合成气提供了一种高效可持续的体系。
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引用次数: 0
UV-activated, high-temperature hydrogen sensing using a single Pd/SiC@C core-shell nanowire: Synergistic enhancement via plasmonic resonance and confinement effect 使用单个Pd/SiC@C核壳纳米线的紫外线激活高温氢传感:通过等离子共振和约束效应的协同增强
IF 9.2 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-07-22 Epub Date: 2026-06-27 DOI: 10.1016/j.ijhydene.2026.156267
Rao Zhang, Guodong Wei, Yudan Qin, Pengyue Liu, Liping Ding, Ruihong Wang, Bei Chen, Pan Wang
To address the high-temperature degradation of conventional Pd-based hydrogen sensors, this study proposes a Pd/SiC@C core-shell nanowire heterostructure. Under UV irradiation, the localized surface plasmon resonance effect in Pd nanoparticles significantly enhances hydrogen adsorption and diffusion. At 300 °C, the sensor achieves a response of 27% to 20 ppm H2, with response and recovery times of 3.5 s and 6.2 s, respectively. It maintains high sensitivity across a wide operating temperature range (50-300 °C) and H2 concentration range (20-200 ppm). Notably, after 30 consecutive days of operation at 300 °C, the device exhibits negligible performance degradation. First-principles calculations confirm strong H2 adsorption and significant interfacial charge transfer at the Pd(111)/SiC(111) interface, supporting the proposed electronic sensitization mechanism. This work establishes a robust design strategy for high-temperature, high-performance hydrogen sensors.
为了解决传统钯基氢传感器的高温降解问题,本研究提出了一种钯/SiC@C核壳纳米线异质结构。在紫外线照射下,局部表面等离子体共振效应显著增强了钯纳米粒子对氢的吸附和扩散。在300 °C时,传感器对20 ppm H2的响应为27%,响应时间和恢复时间分别为3.5 s和6.2 s。它在宽工作温度范围(50-300 °C)和H2浓度范围(20-200 ppm)内保持高灵敏度。值得注意的是,在300 °C下连续运行30天后,该设备的性能下降可以忽略不计。第一性原理计算证实了Pd(111)/SiC(111)界面上的强H2吸附和显著的界面电荷转移,支持了所提出的电子敏化机制。这项工作为高温、高性能氢传感器建立了一个强大的设计策略。
{"title":"UV-activated, high-temperature hydrogen sensing using a single Pd/SiC@C core-shell nanowire: Synergistic enhancement via plasmonic resonance and confinement effect","authors":"Rao Zhang,&nbsp;Guodong Wei,&nbsp;Yudan Qin,&nbsp;Pengyue Liu,&nbsp;Liping Ding,&nbsp;Ruihong Wang,&nbsp;Bei Chen,&nbsp;Pan Wang","doi":"10.1016/j.ijhydene.2026.156267","DOIUrl":"10.1016/j.ijhydene.2026.156267","url":null,"abstract":"<div><div>To address the high-temperature degradation of conventional Pd-based hydrogen sensors, this study proposes a Pd/SiC@C core-shell nanowire heterostructure. Under UV irradiation, the localized surface plasmon resonance effect in Pd nanoparticles significantly enhances hydrogen adsorption and diffusion. At 300 °C, the sensor achieves a response of 27% to 20 ppm H<sub>2</sub>, with response and recovery times of 3.5 s and 6.2 s, respectively. It maintains high sensitivity across a wide operating temperature range (50-300 °C) and H<sub>2</sub> concentration range (20-200 ppm). Notably, after 30 consecutive days of operation at 300 °C, the device exhibits negligible performance degradation. First-principles calculations confirm strong H<sub>2</sub> adsorption and significant interfacial charge transfer at the Pd(111)/SiC(111) interface, supporting the proposed electronic sensitization mechanism. This work establishes a robust design strategy for high-temperature, high-performance hydrogen sensors.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"253 ","pages":"Article 156267"},"PeriodicalIF":9.2,"publicationDate":"2026-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148529663","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
Understanding the density-dependent hydrogen evolution activity and stability in Pt single-atom catalysts 了解Pt单原子催化剂中密度依赖的析氢活性和稳定性
IF 9.2 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-07-22 Epub Date: 2026-06-28 DOI: 10.1016/j.ijhydene.2026.156199
Qing Liu, Changmin Shi, Lijuan Xue, Dongchao Wang, Xiaolong Li, Feifei Li, Hongmei Liu
Recent studies have highlighted the importance of the densely populated single-atom catalysts (SACs), which possess not only higher mass-specific activity but also an additional type of inter-site interactions. However, an excessively high density of single-atom sites on the support often causes metallic aggregation, while too low density may limit their catalytic efficiency. Thus, it is of great significance to identify a moderate density of single-atom sites that can achieve the maximum catalytic efficiency. Herein, we study the effect of the density of single-atom sites on the electronic structure, stability and HER activity of Pt SACs through first-principles calculations, where Pt single atoms are anchored on the surface of Ni nanoclusters. We rationally design a series of Pt SACs with different numbers and various doping positions of Pt atoms. The results reveal that as the number of Pt atoms increases, the stability of Pt SACs linearly increases, while the Gibbs free-energy change of hydrogen adsorption first increases and then linearly decreases. When the density of Pt atoms reaches a moderate level (PtSAC-Pt6Ni49), the SAC exhibits the optimal HER performance. Furthermore, the underlying mechanisms for density modulation are explained by electronic structure analysis. Significantly, the d-band center and the transferred Bader charges of Pt atoms are proposed as electronic descriptors for HER activity, with the latter providing a more sensitive correlation with HER activity, which will facilitate the strategic design of high-performance densely populated SACs. Finally, we also consider realistic catalytic factors, such as support, solvent effects, defects, and atomic aggregation, and investigate their influence on the HER activity and stability of PtNi SACs.
最近的研究强调了密集的单原子催化剂(SACs)的重要性,它不仅具有更高的质量比活性,而且还具有额外类型的位点间相互作用。然而,载体上的单原子位点密度过高往往会导致金属聚集,而密度过低则会限制其催化效率。因此,确定一个中等密度的单原子位点以达到最大的催化效率具有重要意义。在此,我们通过第一性原理计算研究了单原子位密度对Pt SACs电子结构、稳定性和HER活性的影响,其中Pt单原子锚定在Ni纳米簇的表面。我们合理地设计了一系列不同数量和不同掺杂位置的铂原子SACs。结果表明,随着Pt原子数的增加,Pt SACs的稳定性线性增加,而吸附氢的吉布斯自由能变化先增大后线性减小。当Pt原子密度达到中等水平(PtSAC-Pt6Ni49)时,SAC表现出最佳的HER性能。此外,通过电子结构分析解释了密度调制的潜在机制。值得注意的是,d波段中心和Pt原子转移的Bader电荷被认为是HER活度的电子描述符,后者与HER活度的相关性更敏感,这将有助于高性能高密度sac的战略设计。最后,我们还考虑了现实的催化因素,如载体、溶剂效应、缺陷和原子聚集,并研究了它们对PtNi SACs HER活性和稳定性的影响。
{"title":"Understanding the density-dependent hydrogen evolution activity and stability in Pt single-atom catalysts","authors":"Qing Liu,&nbsp;Changmin Shi,&nbsp;Lijuan Xue,&nbsp;Dongchao Wang,&nbsp;Xiaolong Li,&nbsp;Feifei Li,&nbsp;Hongmei Liu","doi":"10.1016/j.ijhydene.2026.156199","DOIUrl":"10.1016/j.ijhydene.2026.156199","url":null,"abstract":"<div><div>Recent studies have highlighted the importance of the densely populated single-atom catalysts (SACs), which possess not only higher mass-specific activity but also an additional type of inter-site interactions. However, an excessively high density of single-atom sites on the support often causes metallic aggregation, while too low density may limit their catalytic efficiency. Thus, it is of great significance to identify a moderate density of single-atom sites that can achieve the maximum catalytic efficiency. Herein, we study the effect of the density of single-atom sites on the electronic structure, stability and HER activity of Pt SACs through first-principles calculations, where Pt single atoms are anchored on the surface of Ni nanoclusters. We rationally design a series of Pt SACs with different numbers and various doping positions of Pt atoms. The results reveal that as the number of Pt atoms increases, the stability of Pt SACs linearly increases, while the Gibbs free-energy change of hydrogen adsorption first increases and then linearly decreases. When the density of Pt atoms reaches a moderate level <strong>(</strong>Pt<sub>SAC</sub>-Pt<sub>6</sub>Ni<sub>49</sub>), the SAC exhibits the optimal HER performance. Furthermore, the underlying mechanisms for density modulation are explained by electronic structure analysis. Significantly, the d-band center and the transferred Bader charges of Pt atoms are proposed as electronic descriptors for HER activity, with the latter providing a more sensitive correlation with HER activity, which will facilitate the strategic design of high-performance densely populated SACs. Finally, we also consider realistic catalytic factors, such as support, solvent effects, defects, and atomic aggregation, and investigate their influence on the HER activity and stability of PtNi SACs.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"253 ","pages":"Article 156199"},"PeriodicalIF":9.2,"publicationDate":"2026-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148502710","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
Curvature-driven orbital engineering of Co single-atom sites in carbon nanotubes for efficient oxygen reduction 碳纳米管中Co单原子位的曲率驱动轨道工程用于高效氧还原
IF 9.2 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-07-22 Epub Date: 2026-06-27 DOI: 10.1016/j.ijhydene.2026.156185
Hongtao Wu, Qingyun Hu, Ninggui Ma, Jun Fan, Zhanhua Wei
The oxygen reduction reaction (ORR) is crucial for the development of metal-air batteries. This work systematically investigates the curvature-mediated regulation of ORR performance in asymmetrically coordinated single-atom catalysts, CoN3Cl doped carbon nanotube (CoN3Cl@CTB), using first-principles calculations. By analyzing the binding energy, ab initio molecular dynamics, and density of states confirm the robust stability and metallic electronic properties of these catalysts. Within an optimal curvature range (CoN3Cl@CTB (9, 4) to (14, 4)), the catalysts demonstrate superior performance. Notably, CoN3Cl@CTB (14, 4) achieves an ultralow overpotential of 0.27 V, representing an approximately 40% improvement over commercial Pt/C. Further orbital analysis shows that performance enhancement stems from curvature's precise modulation of Co's coordination environment: it optimizes interfacial charge transfer and, critically, modulates Co dxz and dx2−y2 orbitals in a diameter-dependent way, inducing energy gap separation and decoupling their π/σ bonding roles, thus fine-tuning intermediate adsorption energies for ORR. This study provides important theoretical insights for designing high-performance cathode materials for metal-air batteries.
氧还原反应(ORR)对金属-空气电池的发展至关重要。本工作系统地研究了不对称配位单原子催化剂,CoN3Cl掺杂碳纳米管(CoN3Cl@CTB)中ORR性能的曲率调节,使用第一性原理计算。通过对结合能、从头算分子动力学和态密度的分析,证实了这些催化剂的鲁棒稳定性和金属电子性能。在最佳曲率范围内(CoN3Cl@CTB(9,4) ~(14,4)),催化剂表现出优异的性能。值得注意的是,CoN3Cl@CTB(14,4)实现了0.27 V的超低过电位,比商用Pt/C提高了约40%。进一步的轨道分析表明,性能的提高源于曲率对Co配位环境的精确调制:它优化了界面电荷转移,并以直径相关的方式调节了Co dxz和dx2−y2轨道,诱导了能隙分离和π/σ键作用的解耦,从而微调了ORR的中间吸附能。该研究为设计高性能金属-空气电池正极材料提供了重要的理论见解。
{"title":"Curvature-driven orbital engineering of Co single-atom sites in carbon nanotubes for efficient oxygen reduction","authors":"Hongtao Wu,&nbsp;Qingyun Hu,&nbsp;Ninggui Ma,&nbsp;Jun Fan,&nbsp;Zhanhua Wei","doi":"10.1016/j.ijhydene.2026.156185","DOIUrl":"10.1016/j.ijhydene.2026.156185","url":null,"abstract":"<div><div>The oxygen reduction reaction (ORR) is crucial for the development of metal-air batteries. This work systematically investigates the curvature-mediated regulation of ORR performance in asymmetrically coordinated single-atom catalysts, CoN<sub>3</sub>Cl doped carbon nanotube (CoN<sub>3</sub>Cl@CTB), using first-principles calculations. By analyzing the binding energy, ab initio molecular dynamics, and density of states confirm the robust stability and metallic electronic properties of these catalysts. Within an optimal curvature range (CoN<sub>3</sub>Cl@CTB (9, 4) to (14, 4)), the catalysts demonstrate superior performance. Notably, CoN<sub>3</sub>Cl@CTB (14, 4) achieves an ultralow overpotential of 0.27 V, representing an approximately 40% improvement over commercial Pt/C. Further orbital analysis shows that performance enhancement stems from curvature's precise modulation of Co's coordination environment: it optimizes interfacial charge transfer and, critically, modulates Co <span><math><mrow><msub><mi>d</mi><mrow><mi>x</mi><mi>z</mi></mrow></msub></mrow></math></span> and <span><math><mrow><msub><mi>d</mi><mrow><msup><mi>x</mi><mn>2</mn></msup><mo>−</mo><msup><mi>y</mi><mn>2</mn></msup></mrow></msub></mrow></math></span> orbitals in a diameter-dependent way, inducing energy gap separation and decoupling their <em>π</em>/<em>σ</em> bonding roles, thus fine-tuning intermediate adsorption energies for ORR. This study provides important theoretical insights for designing high-performance cathode materials for metal-air batteries.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"253 ","pages":"Article 156185"},"PeriodicalIF":9.2,"publicationDate":"2026-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148502678","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
Corrigendum to ‘Adaptive model predictive control for PEM electrolysis system with pre-regulated temperature and pressure approach’ [Int J Hydrogen Energy, 238 (2026), 155160] “预调节温度和压力方法的PEM电解系统的自适应模型预测控制”的更正[J] .氢能源,238 (2026),155160]
IF 9.2 2区 工程技术 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-07-22 Epub Date: 2026-07-01 DOI: 10.1016/j.ijhydene.2026.156038
Jie Song, Zheng Zong, Danxi Liang, Yunxi Yang, Guizhi Xu, Mengyuan Yang, Shaojie Ke, Yanmin Zu, Lixiao Liang, Gendi Li, Chao Xu
{"title":"Corrigendum to ‘Adaptive model predictive control for PEM electrolysis system with pre-regulated temperature and pressure approach’ [Int J Hydrogen Energy, 238 (2026), 155160]","authors":"Jie Song,&nbsp;Zheng Zong,&nbsp;Danxi Liang,&nbsp;Yunxi Yang,&nbsp;Guizhi Xu,&nbsp;Mengyuan Yang,&nbsp;Shaojie Ke,&nbsp;Yanmin Zu,&nbsp;Lixiao Liang,&nbsp;Gendi Li,&nbsp;Chao Xu","doi":"10.1016/j.ijhydene.2026.156038","DOIUrl":"10.1016/j.ijhydene.2026.156038","url":null,"abstract":"","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"253 ","pages":"Article 156038"},"PeriodicalIF":9.2,"publicationDate":"2026-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148502781","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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International Journal of Hydrogen Energy
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