Engineering 3d–2p–4f Gradient Orbital Coupling to Enhance Electrocatalytic Oxygen Reduction

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(42)

Published: Sept. 10, 2022

The development of highly efficient and economical materials for the oxygen reduction reaction (ORR) plays a key role in practical energy conversion technologies. However, intrinsic scaling relations exert thermodynamic inhibition on realizing active ORR electrocatalysts. Herein, novel feasible gradient orbital coupling strategy tuning performance through construction Co 3d-O 2p-Eu 4f unit sites Eu2 O3 -Co model is proposed. Through coupling, pristine ionic property between Eu O atoms assigned with increased covalency, which optimizes eg occupancy sites, weakens OO bond, thus ultimately breaking relation *OOH *OH at Co-O-Eu sites. optimized catalyst displays onset half-wave potential 1.007 0.887 V versus reversible hydrogen electrode, respectively, are higher than those commercial Pt/C most Co-based catalysts ever reported. In addition, found to possess superior selectivity durability. It also reveals better cell noble-metal Zn-air batteries terms high power/energy densities long cycle life. This study provides new perspective electronic modulation by 3d-2p-4f coupling.

Language: Английский

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Heteroatom‐Driven Coordination Fields Altering Single Cerium Atom Sites for Efficient Oxygen Reduction Reaction

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(28)

Published: April 4, 2023

For current single-atom catalysts (SACs), modulating the coordination environments of rare-earth (RE) single atoms with complex electronic orbital and flexible chemical states is still limited. Herein, cerium (Ce) SAs supported on a P, S, N co-doped hollow carbon substrate (Ce SAs/PSNC) for oxygen reduction reaction (ORR) are reported. The as-prepared Ce SAs/PSNC possesses half-wave potential 0.90 V, turnover frequency value 52.2 s

Language: Английский

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Sliding ferroelectricity in van der Waals layered γ-InSe semiconductor

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Jan. 3, 2023

Abstract Two-dimensional (2D) van-der-Waals (vdW) layered ferroelectric semiconductors are highly desired for in-memory computing and photovoltaics or detectors. Beneficial from the weak interlayer vdW-force, controlling structure by twist/translation doping is an effective strategy to manipulate fundamental properties of 2D-vdW semiconductors, which has contributed newly-emerging sliding ferroelectricity. Here, we report unconventional room-temperature ferroelectricity, both out-of-plane in-plane, in vdW-layered γ-InSe semiconductor triggered yttrium-doping (InSe:Y). We determine piezoelectric constant ∼7.5 pm/V InSe:Y flakes with thickness ∼50 nm, about one order magnitude larger than earlier reports. directly visualize enhanced switchable polarization originating fantastic microstructure modifications including stacking-faults elimination a subtle rhombohedral distortion due intralayer compression continuous pre-sliding. Our investigations provide new freedom degrees manipulation intrinsic 2D-vdW-layered expand candidates next-generation nanoelectronics.

Language: Английский

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Rare‐Earth Single‐Atom Catalysts: A New Frontier in Photo/Electrocatalysis

Small Methods, Journal Year: 2022, Volume and Issue: 6(8)

Published: June 25, 2022

Abstract Single‐atom catalysts (SACs) provide well‐defined active sites with 100% atom utilization, and can be prepared using a wide range of support materials. Therefore, they are attracting global attention, especially in the fields energy conversion storage. To date, research has focused on transition‐metal precious‐metal‐based SACs. More recently, rare‐earth (RE)‐based SACs have emerged as new frontier photo/electrocatalysis owing to their unique electronic structure arising from spin‐orbit coupling 4f valence orbitals, unsaturated coordination environment, behavior charge‐transport bridges. However, systematic review role RE sites, catalytic mechanisms, synthetic methods for is lacking. this review, latest developments having applications summarized discussed. First, theoretical advantages briefly introduced, focusing roles orbitals coupled levels. In addition, most recent progress several important photo/electrocatalytic reactions corresponding mechanisms Further, strategies production reported. Finally, challenges development highlighted, along future directions perspectives.

Language: Английский

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Recent Progress in Inorganic Afterglow Materials: Mechanisms, Persistent Luminescent Properties, Modulating Methods, and Bioimaging Applications

Advanced Optical Materials, Journal Year: 2023, Volume and Issue: 11(11)

Published: Jan. 8, 2023

Abstract Persistent luminescence (PL) is a distinctive optical phenomenon with long‐lasting afterglow emissions after the cessation of excitation, thus emerging huge prospects in applications anti‐counterfeiting, information or data storage, photocatalysis, sensing, and bioimaging. In this regard, it great importance to optimize PL performance. Recently, no comprehensive literature review on inorganic persistent phosphors reported aid researchers focusing systematic adjustment properties based progress made recent ten years. Accordingly, motivation work that are interest for dopant host selection criteria, intensity, multi‐color modulating methods, from perspectives composition optimization, defect engineering, coordination environment hosts. Then, X‐ray, light emitting diode (LED), ultraviolet (UV), near‐infrared (NIR) excited imaging multimodal introduced. Finally, summary, challenge, outlook, future development direction field provided. With profound influence materials, believed will be guideline design, synthesis, performance optimization materials future.

Language: Английский

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A review on recent applications and future prospects of rare earth oxides in corrosion and thermal barrier coatings, catalysts, tribological, and environmental sectors

Ceramics International, Journal Year: 2022, Volume and Issue: 48(22), P. 32588 - 32612

Published: July 31, 2022

Language: Английский

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Halide Double Perovskite Nanocrystals Doped with Rare‐Earth Ions for Multifunctional Applications

Advanced Science, Journal Year: 2023, Volume and Issue: 10(20)

Published: April 28, 2023

Most lead-free halide double perovskite materials display low photoluminescence quantum yield (PLQY) due to the indirect bandgap or forbidden transition. Doping is an effective strategy tailor optical properties of materials. Herein, efficient blue-emitting Sb3+ -doped Cs2 NaInCl6 nanocrystals (NCs) are selected as host, rare-earth (RE) ions (Sm3+ , Eu3+ Tb3+ and Dy3+ ) incorporated into excellent PLQY 80.1% obtained. Femtosecond transient absorption measurement found that RE not only served activator but also filled deep vacancy defects. Anti-counterfeiting, thermometry, white-light-emitting diodes (WLEDs) exhibited using these ions-doped NCs. For thermometry based on Sm3+ :Sb3+ NCs, maximum relative sensitivity 0.753% K-1 which higher than those most temperature-sensing Moreover, WLED fabricated by NCs@PMMA displays CIE color coordinates (0.30, 0.28), a luminous efficiency 37.5 lm W-1 CCT 8035 K, CRI over 80, indicate NCs promising single-component phosphors for next-generation lighting technologies.

Language: Английский

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Macroscopic Assembly of Chiral Hydrogen‐bonded Metal‐free Supramolecular Glasses for Enhanced Color‐tunable Ultralong Room Temperature Phosphorescence

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(28)

Published: May 12, 2023

Glassy materials, with desirable mechanical rigidity, shaping ability, high transparency, are attracting great interest in diverse fields. However, optically bulk molecule-based glasses still rare, mainly due to limited monomeric species and harsh preparation conditions. Herein, we report a facile bottom-up solution fabrication process obtain metal-free supramolecular (SMGs) at the macroscopic scale using L-Histidine hexamethylenetetramine as building blocks. The chiral SMGs possess color-tunable ultralong room temperature phosphorescence (decay lifetime up 141.2 ms) circular polarized luminescence (g factor 8.7×10-3 ). strong hydrogen bonds effectively drive formation of SMGs, provide rigid microenvironment boost triplet exciton generation. By virtue excitation- temperature-dependent applications including multicolored displays, visual UV detection, persistently luminescent thermometer demonstrated.

Language: Английский

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Terbium-induced cobalt valence-band narrowing boosts electrocatalytic oxygen reduction

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(11), P. 5500 - 5512

Published: Jan. 1, 2023

Tb 2 O 3 endows Co 3d with a narrow band and appropriate location via 3d–O 2p–Tb 4f gradient orbital coupling to efficiently enhance the oxygen reduction reaction.

Language: Английский

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Rare earth-based nanomaterials in electrocatalysis

Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 489, P. 215204 - 215204

Published: May 3, 2023

Language: Английский

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