B/MoS2中相变辅助光、电、光电催化析氢─机理洞察

IF 7.2 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Chemistry of Materials Pub Date : 2025-05-13 DOI:10.1021/acs.chemmater.4c03268

Daria Baranowska, Tomasz Kędzierski, Grzegorz Leniec, Beata Zielińska, Ewa Mijowska

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引用次数: 0

摘要

电催化水分解是公认的最有效的可持续制氢方法之一，可见光集成最近成为一种有前途的增强策略。为了解决这个问题，我们开发了硼罗芬和二硫化钼（B/MoS2）的2D/2D异质结构，以研究其在酸性条件下光（photo），电（HER）和光电（PEC）催化析氢反应中的效率。优化mos2与硼的质量比可以显著降低过电位，在PEC中达到281.1 mV， Tafel斜率为56.0 mV/dec，而在传统HER中为312.5 mV和160.9 mV/dec，这表明氢的活性和动力学得到了提高。此外，在10 mA/cm2恒定电流密度下的长期稳定性测试证实了B/MoS2的高耐久性，并保持了长达120小时的稳定性能。在PEC中，B/MoS2的析氢速率达到了~ 2.5 mol/g，与原始MoS2相比，分别在光电、电和光催化析氢过程中提高了1.4倍、1.8倍和3152倍。此外，综合材料表征阐明了潜在的PEC机制，包括原位和非原位分析。该研究强调了硼罗芬富集的MoS2作为太阳能和/或电力驱动制氢的高效催化剂的潜力，证实了硼罗芬的存在通过产生应变和缺陷，破坏2H相的稳定，有利于1T相的形成，从而大大促进了MoS2的2H到1T相的转变，从而显著提高了催化性能。有趣的是，在光催化、电催化和光电催化析氢反应中，MoS2的2h - 1t相变都被检测到。然而，其效率遵循以下顺序：PEC >；她比;照片表明可见光照射是一个缺失的活动描述符，揭示了PEC水分裂过程中氢演化机制的谜题。

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Phase Transition Assisted Photo-, Electro- and Photoelectrocatalytic Hydrogen Evolution in B/MoS2─Mechanistic Insight

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Phase Transition Assisted Photo-, Electro- and Photoelectrocatalytic Hydrogen Evolution in B/MoS2─Mechanistic Insight

Electrocatalytic water splitting is recognized as one of the most effective methods for sustainable hydrogen production, with visible light integration recently emerging as a promising enhancement strategy. To address this, we developed a 2D/2D heterostructure of borophene and molybdenum disulfide (B/MoS₂) to investigate its efficiency in photo-(photo), electro-(HER), and photoelectro-(PEC) catalytic hydrogen evolution reactions under acidic conditions. Optimizing the MoS₂-to-boron mass ratio revealed significantly reduced overpotential, achieving 281.1 mV and a Tafel slope of 56.0 mV/dec in PEC, compared to 312.5 mV and 160.9 mV/dec in conventional HER, indicating boosted activity and kinetics of the hydrogen evolution process. Additionally, a long-term stability test at a constant current density of 10 mA/cm² confirmed the high durability of B/MoS₂ and maintained stable performance for up to 120 h. The B/MoS₂ demonstrated an improved hydrogen evolution rate reaching ∼2.5 mol/g in PEC, representing a 1.4-fold, 1.8-fold, and 3152-fold increase compared to pristine MoS₂ in photoelectro-, electro-, and photocatalytic hydrogen evolution process, respectively. Moreover, comprehensive material characterization elucidated the underlying PEC mechanism, including in situ and ex situ analyses. It highlighted the potential of borophene-enriched MoS₂ as an efficient catalyst for solar and/or electricity-driven hydrogen production, confirming that borophene presence substantially promotes the 2H-to-1T phase transition of MoS₂ by creating strain and defects, destabilizing the 2H phase, and favoring the formation of the 1T phase, thus significantly enhancing catalytic performance. Interestingly, the 2H-to-1T phase transition of MoS₂ is detected in all three processes: photo-, electro-, and photoelectrocatalytic hydrogen evolution reactions. However, its efficiency follows the order: PEC > HER > photo indicating that visible light irradiation is a missing activity descriptor revealing a puzzle of hydrogen evolution mechanism during PEC water splitting.

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来源期刊

Chemistry of Materials 工程技术-材料科学：综合

CiteScore

14.10

自引率

5.80%

发文量

929

审稿时长

1.5 months

期刊介绍： The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.