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JOURNAL OF ALLOYS AND COMPOUNDS · 2025 · IF 6.3

Oxygen Vacancy-Rich Ti2NTix MXene as a High-Efficiency Catalyst for Enhanced Hydrogen Desorption of MgH2

Lina Qin,Guorong Zhang,Taigen Liang,Lixian Sun,Fen Xu,Yongpeng Xia,Sergey P. Verevkin,Sergey V. Vostrikov,Anton Lvovich Maximovi,Xuezhang Xiao,Lixin Chen,Hongge Pan

As a prominent catalyst in the development of MgH 2 hydrogen storage materials, MXene can significantly enhance hydrogen storage performance. In this study, we investigated the impact of using molten salts instead of HF to treat Ti 2 NTi x and its impact on the hydrogen storage properties of MgH 2 . MgH 2 -10 wt% Ti 2 NTi x composite has been prepared via ball milling. The results showed that adding 10   wt% Ti 2 NTi x largely lowered the initial dehydrogenation temperature of MgH 2 from 300.2 ℃ to 173.5 ℃. Under isothermal conditions at 350 ℃, the composite released 6.11   wt% H 2 within 4   minutes. Furthermore, after dehydrogenation, the MgH 2 -10 wt% Ti 2 NTi x composite absorbed 3.4   wt% H 2 in 60   minutes at 100 ℃ and 30   bar hydrogen pressure. EPR found that there is a large number of oxygen vacancies on the Ti 2 NTi x surface introduced by molten salt treatment, providing abundant active sites and accelerating electron transfer. Additionally, the in-situ formation of titanium nitride compounds, the synergistic multivalent catalytic effect of titanium, and the multiphase interfaces in MgH 2 -10 wt% Ti 2 NTi x contributed to the composite’s improved catalytic activity and stability. This work provided valuable insights into the application of oxygen vacancy-rich, incompletely etched Ti 2 NTi x materials in magnesium-based hydrogen storage, demonstrating their great potential in hydrogen storage technologies.

CAS / MDL: 7789-23-3 7789-24-4
研究领域: 材料科学 · 能源存储
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2022 · IF 7.139

Insight into the mechanism of hydrogen permeation inhibition by cerium during electroplating: Enhanced kinetics of hydrogen desorption

Pengyuan Zhang,Zhengyi Xu,Bo Zhang,Bing Lei,Zhiyuan Feng,Guozhe Meng,Yanqiu Wang,Junyi Wang,Fuhui Wang

In our previous work, we found that hydrogen permeation can be noticeably reduced during Ni–Cu electroplating by the addition of Ce salt to the plating solution. The mechanism of hydrogen permeation inhibition via Ce salt was further studied in the present work. Through the Iver–Pickering–Zamenzadeh (IPZ) model fitting of the kinetic of hydrogen evolution reaction , we found that the trace Ce salt that precipitated during electroplating could improve Tafel reaction kinetic parameters and reduce the strength of the Ni–H and Cu–H bonds due to its abundant d/f electrons and enough d/f orbitals. Meanwhile, Ce can provide electrons for the Heyrovsky reaction. These effects promoted surface electron migration and thus led to the desorption of adsorbed hydrogen atoms (H ads ) and the decreased diffusion of H ads into the Ni–Cu coatings. The accuracy of the IPZ model fitting results was verified by hydrogen evolution rate experiments during the electroplating process. Hence, Ce salt can effectively inhibit hydrogen permeation and reduce the dehydrogenation annealing time, thereby showing great potential for energy saving and emission reduction in the electroplating industry.

研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2019 · IF 8.456

Design Superior Alkaline Hydrogen Evolution Electrocatalyst by Engineering Dual Active Sites for Water Dissociation and Hydrogen Desorption

Jianpo Chen,Qiuyan Jin,Yinwei Li,Yan Li,Hao Cui,Chengxin Wang

In alkaline media, the water-dissociation-related Volmer process always suppresses the hydrogen formation/desorption process, which makes it challenging to develop non-noble-metal alkaline electrocatalysts with excellent catalytic activity. Here, we proposed a two-pronged strategy to simultaneously promote the kinetic process of both water dissociation and hydrogen desorption with the Co-doped WO2/amorphous CoxW hybrid electrocatalyst. Impressively, the optimized hybrid exhibits an outstanding hydrogen evolution reaction (HER) activity with the quite small Tafel slope of 19.77 mV dec–1 and ultralow overpotential of just 25 mV to reach a current density of 10 mA cm–2 in alkaline media. Both experiments and density functional theory calculations reveal that the top-level HER performance can be attributed to the cooperation of two different active components, in which the water molecule can easily be activated on the amorphous CoxW with low energy barrier (ΔGw = 0.46 eV), while hydrogen atoms can rapidly desorb from the Co-doped WO2 with an optimal Gibbs free energy of hydrogen adsorption (ΔGH* = −0.06 eV). Also, the density functional theory calculation further confirms that the H* tends to combine with another H* via Tafel step rather than Heyrovsky step. The findings provide unique insights for the development of the state-of-the-art non-noble-metal HER electrocatalyst with a Pt-like kinetic behavior in alkaline media.

研究领域: 材料科学 · 电化学
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY · 2025 · IF 14.3

Effects of spark plasma sintering parameters on sintering mechanism of yttrium hydride

Xuyang Shang,Yuxin Lin,Keke Hou,Yajuan Zhong,Changqing Cao,Yanhui Wang,Hongtao Zeng,Jun Lin

Yttrium hydride (YH x ) is a highly promising neutron moderator material for nuclear reactors, known for its exceptional thermal stability and high hydrogen content. This study investigated the sintering mechanism and microstructural evolution of YH x monoliths processed by spark plasma sintering (SPS), with the effects of temperature, duration, and pressure. The results indicate that the sintering process can be divided into five stages: formation of sintering necks, rapid densification, anti-densification, recrystallization, and grain growth. The anti-densification behavior is attributed to hydrogen desorption, phase transformation-induced volumetric contraction, and vacancy coalescence from hydrogen migration, leaving residual pores and lattice defects. Furthermore, increasing the sintering temperature and duration promotes recrystallization and grain growth, whereas elevated pressure effectively suppresses grain boundary migration. This research establishes fundamental processing-structure correlations critical for optimizing YH x moderators in nuclear applications.

研究领域: 材料科学 · 核能工程
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Inorganic Chemistry Frontiers · 2025 · IF 6.4

Ultraviolet light-induced carbon defects on MOF-derived Ni@C with greatly improved electrocatalytic activity in hydrogen evolution

Ting Wu,Jianpeng Sun,Zhan Zhao,Kelei Huang,Xiangchao Meng

Modulation of d-band center of Ni to achieve an equilibrium between H-adsorption and Hdesorption (H ads /H des ) remains a great challenge. Herein, Ni@C derived from MOFs was treated by ultraviolet light. It was found that sp 2 edge carbon were converted to sp 3 defective carbon and further combined with Ni clusters. Experimental and theoretical calculations confirmed that the enhanced d-p orbital hybridization between C-Ni promoted a large negative shift of the dband center of Ni, which was in favor of improving the HER activity of the catalyst. Moreover, the core-shell structure of carbon-coated Ni effectively protected the Ni sites and improved its catalytic stability when applied in electrocatalytic water splitting. As a result, as-prepared UV-Ni@C/NF exhibited excellent HER activity in both alkaline aqueous solution (overpotential of 309 mV at 1000 mA cm -2 ) and acidic aqueous solution (overpotential of 446 mV at 1000 mA cm -2 ). This study indicated the UV-illumination-induced defects method as a feasible strategy to precisely regulate the d-band center of Ni.

研究领域: 材料科学 · 电化学 · 纳米技术 · 催化 · 能量转换
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Advanced Energy Materials · 2025 · IF 26

Single-Atom Catalysts with Microenvironment Tuned by High Entropy for Efficient and Stable Alkaline Hydrogen Evolution Reaction

Bangxin Li,Mingyue Yuan,Yihao Liu,Jinwen Zhang,Yuting Miao,Xuhui Xiong,Jiachen Sun,Renchao Che,Heyong He

Conventional non-noble hydrogen evolution reaction catalysts are plagued by excessive hydrogen adsorption and instability. To overcome this, we pioneer a high-entropy single-atom (HESA) catalyst via precise anchoring of multiple transition metals on carbon supports. The HESA catalyst achieves record-breaking alkaline HER performance of 44 mV@10 mA cm −2 (matching commercial Pt/C catalyst) and 300 h stability, resolving the persistent activity-stability trade-off. Systematical characterizations reveal that low-coordination metal sites induce significant metal-support charge redistribution. Electronegative supports withdraw electrons from metal centers, while π-back-donation downshifts metal d-band centers, optimizing the Gibbs free energy of intermediate H atoms (ΔG H* ). Atomic-scale imaging further confirms uniform charge distribution and Ångström-level electric field response. Crucially, adjacent multi-metal sites synergistically lower energy barriers for both water dissociation and hydrogen desorption through a synergistic electronic buffering effect. This work establishes entropy-driven microenvironment engineering as a paradigm for cooperative optimization of active sites and electronic structures, opening avenues for durable non-precious catalysts.

研究领域: 催化 · 材料科学 · 电化学 · 能量转换 · 纳米技术
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Journal of Materials Chemistry A · 2024 · IF 10.7

Enhanced photocatalytic H2 evolution: optimized atomic hydrogen desorption via free-electron transfer in sulfur-rich MoWS2+x on vacancy-engineered CdS crystals

Ruiding Fei,Jianfeng Zhao,Huinan Wang,Huijuan Lin,Kui Xu,Guang Zeng,Wenchao Wang,Zhiping Yan

The hydrogen evolution capacity of MoS2 is impeded by its intrinsically highly electronegative sulfur sites, which firmly bind absorbed atomic H through S–Hads bonds and subsequently diminish H2 release. Designing effective surface-active sites to optimize atomic hydrogen activation and desorption for the hydrogen evolution reaction (HER) in water, while also expanding near-infrared (NIR) light responsiveness, remains a significant challenge. We have developed complexes of sulfur vacancy (Sv) enriched CdSv capped with W-modified MoS2+x (MoWS2+x) through an in situ substitution approach, followed by a photoreduction reaction. The bimetallic MoWS2+x cocatalyst not only increases the density of unsaturated coordinating S active sites but also attenuates the strength of the S–Hads bond. The optimized MoWS2+x/CdSv hybrid shows synergistic improvement of atomic H activation and desorption for the solar-driven HER, achieving the highest recorded H2-evolution rate of 9166.13 μmol g−1 h−1 under visible light (λ ≥ 420 nm), which marks a substantial improvement (greater than 750%), and an apparent quantum yield of 19.13%. Remarkably, the target photocatalyst, which is abundant in sulfur vacancies within its CdSv component, also achieves H2 production driven by NIR light beyond 780 nm, with a H2 evolution rate of 1326.82 μmol g−1 h−1. Comprehensive experimental and theoretical investigations corroborate that the existence of unsaturated coordinated S sites mitigates the strength of S–Hads bonds, resulting in the high driving force of H2 bubble release from water and long-lived active charge carriers. In this paper, we constructed visible light and NIR-active photocatalysts successfully for hydrogen production, highlighting the synergetic effects within this unique system. Additionally, the photo-behaviors of charge carriers have been investigated by ultra-fast spectroscopic techniques to gain a deeper understanding of the interfacial charge transfer kinetics. This study provides valuable insights into the development and optimization of photocatalysts that are responsive to both NIR and visible light, paving the way for more efficient solar-driven applications.

研究领域: 材料科学 · 催化 · 光化学 · 可再生能源
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