Enhanced hydrogen evolution of single-atom Ru sites via geometric and electronic engineering: N and S dual coordination

Wang, Min Jie; Ji, Muwei; Zheng, Xingqun; Jiang, Chi; Zhao, Hang; Mao, Zhiping; Zhang, Minghui; Zhu, Caizhen; Xu, Jian

doi:10.1016/j.apsusc.2020.148742

Cited by 21 publications

(13 citation statements)

References 44 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…47 In contrast, these peaks exhibit the obvious offset toward the high binding energy. 48 It implies the effective electron transfer from the PCN skeleton to Ru atoms through the formed Ru−N bonds, which is also confirmed by the negative shift of Ru 3p XPS of PCN-Ru relative to the reported peaks (Figure S3b). 49,50 The robust Ru−N bonds formed between the adjacent two melon strands suggest the improved in-plane charge transfer ability and superior stability to propel the PHE performance.…”

Section: ■ Results and Discussionsupporting

confidence: 59%

“…N 1s XPS of PCN in Figure b shows three peaks at 398.4, 399.4, and 400.9 eV, which are indexed to sp 2 -hybridized nitrogen (N–CN/C–NC), tertiary nitrogen (N–C 3 ), and terminal amino groups (C–NH 2 ), respectively . In contrast, these peaks exhibit the obvious offset toward the high binding energy . It implies the effective electron transfer from the PCN skeleton to Ru atoms through the formed Ru–N bonds, which is also confirmed by the negative shift of Ru 3p XPS of PCN-Ru relative to the reported peaks (Figure S3b).…”

Section: Resultsmentioning

confidence: 82%

See 1 more Smart Citation

Synergies of Adjacent Sites in Atomically Dispersed Ruthenium toward Achieving Stable Hydrogen Evolution

et al. 2022

Inorg. Chem.

View full text Add to dashboard Cite

It is a challenge to fabricate atomically dispersed metal clusters in polymeric carbon nitride (PCN) for durable photocatalytic reactions owing to the thermodynamic stability limitation. Herein, atomically dispersed Ru clusters are implanted into the PCN skeleton matrix based on an ionic diffusion and coordination (IDC) strategy, the stability of which is improved owing to the robust Ru−N bonds in the formed RuN 4 and RuN 3 configurations. Additionally, RuN 4 and RuN 3 as charge transport bridges between two adjacent melon strands efficaciously conquer hydrogen bond restriction in the skeleton to facilitate the in-plane mobility and separation of charge carriers. Moreover, the synergistic effect of adjacent Ru atoms is triggered on the assembled RuN 3 −RuN 4 and RuN 3 −RuN 3 in the atomically dispersed Ru clusters to significantly decrease hydrogen adsorption energy. As a result, the optimal PCN-Ru photocatalyst achieves nearly 6 times higher than the photocatalytic hydrogen evolution (PHE) rate of the Pt/PCN benchmark and maintains the long-term stable running for 104 h of 26 cycles; its overall PHE performance is far superior to the most of single atoms supported on g-C 3 N 4 photocatalysts reported. The findings here gain new insight into the preparation strategy, structure configuration, and reaction mechanism for atomically dispersed metal clusters supported on PCN, which further stimulates the intensive investigations toward developing more efficient and stable PCN-like photocatalytic materials.

show abstract

Section: ■ Results and Discussionsupporting

confidence: 59%

Section: Resultsmentioning

confidence: 82%

Synergies of Adjacent Sites in Atomically Dispersed Ruthenium toward Achieving Stable Hydrogen Evolution

et al. 2022

Inorg. Chem.

View full text Add to dashboard Cite

show abstract

“…Generally speaking, the electronic structure of the active site is regulated by introducing different heteroatoms to anchor the metal single atoms, so as to optimize the catalyst performance. − Based on the existing research, the tetracoordinate pyridine-N substrate may have the best catalytic activity and the commonly used heteroatoms are B, N, , O, P, − S, − etc. However, in view of the existence of S poisoning in the acetylene hydrochlorination reaction, in this work, we constructed a CuX 4 (X = B, C, N, O, P) catalytic site, and explored the detailed mechanism by DFT calculations.…”

Section: Introductionmentioning

confidence: 99%

Effect of Different Heteroatoms Anchoring a Cu Single-Atom Catalyst on Acetylene Hydrochlorination

et al. 2022

View full text Add to dashboard Cite

A Cu-based catalyst has the advantages of low price and high reserves as well as catalytic activity in acetylene hydrochlorination. In order to better design and prepare efficient Cu single-atom catalysts (SACs) for acetylene hydrochlorination, a single Cu atom anchored by different heteroatoms was investigated by constructing the CuX4 (X = B, C, N, O, P) structure using the spin-polarized density functional theory (DFT). According to the results, the N-doped substrate significantly increased the charge of the Cu atom, and B- and P-doped substrates provided multiple active sites, while the O-doped substrate could not stably anchor the single Cu atom. In general, different catalysts had different dominant mechanisms, and it was found that the charge transfer between single metal atoms and substrates could be used as a descriptor of the catalytic performance. This work reveals the effect mechanisms of the local coordination environment for Cu SACs catalyzing acetylene hydrochlorination, as well as provides theoretical insights for the rational design of efficient Cu-based catalysts.

show abstract

“…The crystal-glass nanodual-phase Al 73 Mn 7 Ru 20 exhibits better HER catalytic performance than the noble metal-based HER catalysts (Fig. 3E) (40,42,45,(48)(49)(50)(51)(52)(53)(54)(55)(56)(57). The current-time curve at 50 mA cm −2 (Fig.…”

Section: Resultsmentioning

confidence: 94%

A crystal glass–nanostructured Al-based electrocatalyst for hydrogen evolution reaction

Liu

Zhong

et al. 2022

Sci. Adv.

View full text Add to dashboard Cite

Platinum-based catalysts are widely used in hydrogen evolution reactions; however, their applications are restricted because of the cost-efficiency trade-off. Here, we present a thermodynamics-based design strategy for synthesizing an Al 73 Mn 7 Ru 20 (atomic %) metal catalyst via combinatorial magnetron co-sputtering. The new electrocatalyst is composed of ~2 nanometers of medium-entropy nanocrystals surrounded by ~2 nanometers of amorphous regions. The catalyst exhibits exceptional performance, similar to that of single-atom catalysts and better than that of nanocluster-based catalysts. We use aluminum rather than a noble metal as the principal element of the catalyst and ruthenium, which is cheaper than platinum, as the noble metal component. The design strategy provides an efficient route for the development of electrocatalysts for use in large-scale hydrogen production. Moreover, the superior hydrogen reaction evolution created by the synergistic effect of the nano-dual-phase structure is expected to guide the development of high-performance catalysts in other alloy systems.

show abstract

Enhanced hydrogen evolution of single-atom Ru sites via geometric and electronic engineering: N and S dual coordination

Cited by 21 publications

References 44 publications

Synergies of Adjacent Sites in Atomically Dispersed Ruthenium toward Achieving Stable Hydrogen Evolution

Synergies of Adjacent Sites in Atomically Dispersed Ruthenium toward Achieving Stable Hydrogen Evolution

Effect of Different Heteroatoms Anchoring a Cu Single-Atom Catalyst on Acetylene Hydrochlorination

A crystal glass–nanostructured Al-based electrocatalyst for hydrogen evolution reaction

Contact Info

Product

Resources

About