Atomic interface regulation of rare-marth metal single atom catalysts for energy conversion

Zhan, Ziheng; Sun, Zhiyi; Wei, Zihao; Li, Yaqiong; Chen, Wenxing; Li, Shenghua; Pang, Siping

doi:10.1007/s12274-023-6287-5

Cited by 9 publications

(2 citation statements)

References 152 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…As shown in Figure 3b, the effect of the crystal field on the rare earth metal ions generally causes Mott transition of the electrons between 4f orbital and outer 5d orbital, then the electron states 4f 6 5d 0 of Sm will be transformed into 4f 5 5d 1 , which will undergo a f-d hybridization in Sm. [35,47] The d-p hybridization between p orbitals of S in LiPSs and d orbitals of metal ions is treated as the primary cause of LiPSs catalytic conversion. Different from transition metal ions, the rare earth element Sm possesses empty 5d orbital and partial occupied 4f orbital.…”

Section: Methodsmentioning

confidence: 99%

“…[33] Recent studies have confirmed that the spin-orbit interaction in rare earth metals can be activated through engineering the single atomic species configuration, resulting in promising electrocatalytic activity. [34,35] The rare earth element of Sm has the electron state of [Xe]4f 6 6s 2 , whose occupied state of 4f orbital is close to the half-full state (7 of 14). Therefor the inner orbitals of Sm is active to occur Mott transition to generate orbital coupling.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Rare Earth Single‐Atom Catalysis for High‐Performance Li−S Full Battery with Ultrahigh Capacity

Zhou,

Ren,

et al. 2024

Angewandte Chemie

View full text Add to dashboard Cite

Lithium‐sulfur (Li−S) batteries have many advantages but still face problems such as retarded polysulfides redox kinetics and Li dendrite growth. Most reported single atom catalysts (SACs) for Li−S batteries are based on d‐band transition metals whose d orbital constitutes active valence band, which is inclined to occur catalyst passivation. SACs based on 4f inner valence orbital of rare earth metals are challenging for their great difficulty to be activated. In this work, we design and synthesize the first rare earth metal Sm SACs which has electron‐rich 4f inner orbital to promote catalytic conversion of polysulfides and uniform deposition of Li. Sm SACs enhance the catalysis by the activated 4f orbital through an f‐d‐p orbital hybridization. Using Sm‐N3C3 modified separators, the half cells deliver a high capacity over 600 mAh g−1 and a retention rate of 84.3% after 2000 cycles. The fabricated S/CNTs|Sm‐N3C3@PP|Sm‐N3C3‐Li full batteries can provide an ultra‐stable cycling performance of a retention rate of 80.6% at 0.2 C after 100 cycles, one of the best full Li−S batteries. This work provides a new perspective for the development of rare earth metal single atom catalysis in electrochemical reactions of Li−S batteries and other electrochemical systems for next‐generation energy storage.

show abstract

Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Rare Earth Single‐Atom Catalysis for High‐Performance Li−S Full Battery with Ultrahigh Capacity

Zhou,

Ren,

et al. 2024

Angewandte Chemie

View full text Add to dashboard Cite

show abstract

Enhancement of Electromagnetic Wave Attenuation through Polarization Loss Induced by Hybridization of Rare‐Earth 4f and Mo‐4d Orbitals in Liquid Plasma

Wen,

Hui,

Chang

et al. 2024

Adv Funct Materials

View full text Add to dashboard Cite

The incorporation of large‐sized rare earth (RE) elements with high coordination characteristics into transition metal dichalcogenide (TMD) absorbers while preserving a high 1T phase content during post‐processing poses a significant challenge. To address this, a novel strategy involving the confinement of RE elements within the 1T‐MoS2 lattice via liquid plasma assistance, is proposed. This approach effectively mitigates the environmental impact on the 1T phase of MoS2, yielding a remarkable 1T phase content of 82.69% for Ce20‐D7 (20 wt.% Cerium trinitrate and 7 kV applied voltage). Combining experimental and theoretical investigations reveals that the multi‐orbital characteristics of RE elements facilitate hybridization between the RE‐4f and Mo‐4d orbitals on the MoS2 surface, leading to the occupation of weakly bound electrons in bonding orbitals with short‐distance motion, enhanced inter‐orbital electron‐electron interactions, and induced polarization loss. Notably, the results demonstrate that the Pr15‐D7 sample (15 wt.% praseodymium nitrate and 7 kV applied voltage) exhibits an effective absorption bandwidth (EAB) of 7.12 GHz at 2.6 mm, with a minimum reflection loss of ‐52.02 dB while the Ce20‐D7 sample achieves an EAB of 6.96 GHz at 2.7 mm. These findings provide valuable insights for the rational design and development of high‐performance TMD absorbers leveraging RE‐modified materials.

show abstract

From Single Atom Photocatalysts to Synergistic Photocatalysts: Design Principles and Applications

Luo,

Wang,

Gao

et al. 2024

Adv Funct Materials

View full text Add to dashboard Cite

Photocatalysis represents a solar‐to‐chemical energy transformation process including three processes, light absorption, charge separation/transfer, and surface reactions. Owing to the merits of single‐atom catalysts (SACs) toward maximal atom utilization, unsaturated coordination structure, and tunable electronic configuration, single‐atom photocatalysts (SAPs) exhibit extraordinary photocatalytic performance toward a series of sustainable reactions. Accompanied by the complexity of photocatalytic processes and the realistic demand for tandem reactions as well as the promotion of intricate reactions with multiple reaction routes and intermediates, significant efforts are desired to gain in‐depth insights into the design and fabrication of synergistic photocatalysts. In this review, the first part discusses the design principles from traditional semiconductor‐based photocatalysts to SAPs. Moreover, six basic models of synergistic photocatalysts including remote dual atoms, bridged dual atoms, adjacent dual atoms, single atoms + clusters/nanoparticles (NPs), single atoms + defects, NPs + NPs, are highlighted and distinguished by their structure features. Second, specific examples of SAPs and synergistic photocatalysts are appreciated under the category of CO2 reduction reaction (CO2RR), hydrogen evolution reaction (HER), nitrogen reduction reaction (NRR), and pollutants degradation. Finally, this review will conclude by discussing the challenges and future perspectives of SAPs and synergistic photocatalysts for sustainable applications.

show abstract

Atomic interface regulation of rare-marth metal single atom catalysts for energy conversion

Cited by 9 publications

References 152 publications

Rare Earth Single‐Atom Catalysis for High‐Performance Li−S Full Battery with Ultrahigh Capacity

Rare Earth Single‐Atom Catalysis for High‐Performance Li−S Full Battery with Ultrahigh Capacity

Enhancement of Electromagnetic Wave Attenuation through Polarization Loss Induced by Hybridization of Rare‐Earth 4f and Mo‐4d Orbitals in Liquid Plasma

From Single Atom Photocatalysts to Synergistic Photocatalysts: Design Principles and Applications

Contact Info

Product

Resources

About