2024 New's Items

Revealing Dynamic Evolution of the Anode-Electrolyte Interphase in All-Solid-State Batteries with Excellent Cyclability

Kim SY
Bak S
Jun K
Ceder G
Chen G
2024

All-solid-state-batteries (ASSBs) based on a halide solid electrolyte (SE) and a lithium-metal based anode typically have poor cyclability without a buffer layer (such as Li3PS4 or Li6PS5Cl) to prevent the degradation reactions. Here excellent cycling stability of ASSB consisting of an uncoated single-crystal LiNi0.8Co0.1Mn0.1O2 cathode and a Li3YCl6 (LYC) SE separator in direct contact with a Li-In anode are demonstrated. Through a combination of...

Selective Synthesis of Defect-Rich LaMnO3 by Low-Temperature Anion Cometathesis

Tran GT
Wustrow A
O’Nolan D
Tao S
Bartel CJ
He T
McDermott MJ
McBride BC
Chapman KW
Billinge SJL
Persson KA
Ceder G
Neilson JR
2024

The synthesis of complex oxides at low temperatures brings forward aspects of chemistry not typically considered. This study focuses on perovskite LaMnO3, which is of interest for its correlated electronic behavior tied to the oxidation state and thus the spin configuration of manganese. Traditional equilibrium synthesis of these materials typically requires synthesis reaction temperatures in excess of 1000 °C, followed by subsequent annealing steps at lower temperatures and different p(O2) conditions to manipulate the oxygen content postsynthesis (e.g., LaMnO...

Fast Room-Temperature Mg-Ion Conduction in Clay-Like Halide Glassy Electrolytes

Yang X
Gupta S
Chen Y
Sari D
Hau H
Cai Z
Dun C
Qi M
Ma L
Liu Y
Urban JJ
Ceder G
2024

The discovery of mechanically soft solid-state materials with fast Mg-ion conduction is crucial for the development of solid-state magnesium batteries. In this paper, novel magnesium gallium halide compounds are reported that achieve high ionic conductivity of 0.47 mS cm−1 at room temperature. These Mg-ion conductors obtained by ball milling Mg and Ga salts exhibit clay-like mechanical properties, enabling intimate contact at the electrode–electrolyte interface during battery cycling. With a combination of experimental and computational analysis, this study identifies that the...

Iron homo- and heterobimetallic complexes supported by a symmetrical dinucleating ligand

Pablo R
See MS
Gonzalez O
Ford RC
Nicolay A
Rao G
Britt RD
Bediako DK
Tilley TD
2024

The selective synthesis of biomimetic Fe/Mn complexes able to mimic the geometry and catalytic activity of enzymes possessing this cofactor is still a challenge. Herein, we discuss the stepwise synthesis, characterization, and magnetic properties of a Fe(II)/Mn(II) species and related Fe(II)/Fe(II) complexes.

The role of manganese in CoMnOx catalysts for selective long-chain hydrocarbon production via Fischer-Tropsch synthesis

Chen H
Lian Z
Zhao X
Wan J
Pieters PF
Oliver-Meseguer J
Yang J
Pach E
Carenco S
Treps L
Liakakos N
Shan Y
Altoe V
Wong E
Zhuo Z
Yang F
Su J
Guo J
Blum M
Lapidus SH
Hunt A
Waluyo I
Ogasawara H
Zheng H
Yang P
Bell AT
López N
Salmeron M
2024

Cobalt is an efficient catalyst for Fischer−Tropsch synthesis (FTS) of hydrocarbons from syngas (CO + H2) with enhanced selectivity for long-chain hydrocarbons when promoted by Manganese. However, the molecular scale origin of the enhancement remains unclear. Here we present an experimental and theoretical study using model catalysts consisting of crystalline CoMnOx nanoparticles and thin films, where Co and Mn are mixed at the sub-nm scale. Employing TEM and in-situ X-ray spectroscopies (XRD, APXPS, and XAS), we determine the catalyst’s atomic structure, chemical...

Particle on a Rod: Surface-Tethered Catalyst on CdS Nanorods for Enzymatically Active Nicotinamide Cofactor Generation

Jayasinghe L
Wei J
Kim J
Lineberry E
Yang P
2024

The photochemical generation of nicotinamide cofactor 1,4- NADH, facilitated by inorganic photosensitizers, emerges as a promising model system for investigating charge transfer phenomena at the interface of semiconductors and bacteria, with implications for enhancing photosynthetic biohybrid systems (PBSs). However, extant semiconductor nanocrystal model systems suffer from achieving optimal conversion efficiency under visible light. This study investigates quasi-one-dimensional CdS nanorods as superior light absorbers, surface modified with catalyst Cp*Rh(4,4′-COOH-bpy)Cl2 to produce...

Dynamic Evolution of Copper Nanowires during CO2 Reduction Probed by Operando Electrochemical 4D-STEM and X‑ray Spectroscopy

Yang Y
Shi C
Feijóo J
Jin J
Chen C
Han Y
Yang P
2024

Nanowires have emerged as an important family of one-dimensional (1D) nanomaterials owing to their exceptional optical, electrical, and chemical properties. In particular, Cu nanowires (NWs) show promising applications in catalyzing the challenging electrochemical CO2 reduction reaction (CO2RR) to valuable chemical fuels. Despite early reports showing morphological changes of Cu NWs after CO2RR processes, their structural evolution and the resulting exact nature of active Cu sites remain largely elusive, which calls for the development of multimodal operando time-resolved nm-scale methods...

A red-light-powered silicon nanowire biophotochemical diode for simultaneous CO2 reduction and glycerol valorization

Kim J
Lin JA
Kim J
Roh I
Lee S
Yang P
2024

A bias-free photochemical diode, in which a p-type photocathode is connected to an n-type photoanode to harness light for driving photoelectrochemical reduction and oxidation pairs, serves as a platform for realizing light-driven fuel generation from CO2. However, the conventional design, in which cathodic CO2 reduction is coupled with the anodic oxygen evolution reaction (OER), requires substantial energy input. Here we present a photochemical diode device that harnesses red light (740 nm) to simultaneously drive biophotocathodic CO2-to-multicarbon conversion and photoanodic glycerol...

Room-Temperature Ferroelectric Epitaxial Nanowire Arrays with Photoluminescence

Le HKD
Zhang Y
Behera P
Vailionis A
Phang A
Brinn R
Yang P
2024

The development of large-scale, high-quality ferroelectric semiconductor nanowire arrays with interesting light-emitting properties can address limitations in traditional wide-bandgap ferroelectrics, thus serving as building blocks for innovative device architectures and next-generation high-density optoelectronics. Here, we investigate the optical properties of ferroelectric CsGeX3 (X = Br, I) halide perovskite nanowires that are epitaxially grown on muscovite mica substrates by vapor phase deposition. Detailed structural characterizations reveal an incommensurate heteroepitaxial...

Complete miscibility of immiscible elements at the nanometre scale

Chen PC
Gao M
McCandler CA
Song C
Jin J
Yang Y
Maulana AL
Persson KA
Yang P
2024

Understanding the mixing behaviour of elements in a multielement material is important to control its structure and property. When the size of a multielement material is decreased to the nanoscale, the miscibility of elements in the nanomaterial often changes from its bulk counterpart. However, there is a lack of comprehensive and quantitative experimental insight into this process. Here we explored how the miscibility of Au and Rh evolves in nanoparticles of sizes varying from 4 to 1 nm and composition changing from 15% Au to 85% Au. We found that the two immiscible elements exhibit a...