2022 New's Items

The Interactive Dynamics of Nanocatalyst Structure and Microenvironment during Electrochemical CO2 Conversion

Yu S
Louisia S
Yang P
2022

In the pursuit of a decarbonized society, electrocatalytic CO2 conversion has drawn tremendous research interest in recent years as a promising route to recycling CO2 into more valuable chemicals. To achieve high catalytic activity and selectivity, nanocatalysts of diverse structures and compositions have been designed. However, the dynamic structural transformation of the nanocatalysts taking place under operating conditions makes it difficult to study active site configurations present during the CO2...

Controlling the Phase Transition in CsPbI3 Nanowires

Lin C-K
Zhang Y
Gao M
Lin J-A
Le HKD
Lin Z
Yang P
2022

Cesium lead iodide (CsPbI3) is a promising semiconductor with a suitable band gap for optoelectronic devices. CsPbI3 has a metastable perovskite phase that undergoes a phase transition into an unfavorable nonperovskite phase in an ambient environment. This phase transition changes the optoelectronic properties of CsPbI3 and hinders its potential for device applications. Therefore, it is of central importance to understand the kinetics of such instability and develop strategies to control and stabilize the...

Photoelectrochemical CO2 Reduction toward Multicarbon Products with Silicon Nanowire Photocathodes Interfaced with Copper Nanoparticles

Roh I
Yu S
Lin C-K
Louisia S
Cestellos-Blanco S
Yang P
2022

The development of photoelectrochemical systems for converting CO2 into chemical feedstocks offers an attractive strategy for clean energy storage by directly utilizing solar energy, but selectivity and stability for these systems have thus been limited. Here, we interface silicon nanowire (SiNW) photocathodes with a copper nanoparticle (CuNP) ensemble to drive efficient photoelectrochemical CO2 conversion to multicarbon products. This integrated system enables CO2-to-C2H...

The presence and role of the intermediary CO reservoir in heterogeneous electroreduction of CO2

Louisia S
Kim D
Li Y
Gao M
Yu S
Roh I
Yang P
2022

Despite the importance of the microenvironment in heterogeneous electrocatalysis, its role remains unclear due to a lack of suitable characterization techniques. Multistep reactions like the electroconversion of CO2 to multicarbons (C2+) are especially relevant considering the potential creation of a unique microenvironment as part of the reaction pathway. To elucidate the significance of the microenvironment during CO2 reduction, we develop on-stream substitution of reactant isotope (OSRI), a method that...

Laser-accelerated phase transformation in cesium lead iodide perovskite

Lin Z
Folgueras MC
Le HKD
Gao M
Yang P
2022

High-temperature phase CsPbI3 has garnered increased attention due to its suitable band gap for photovoltaics, but its structural instability under ambient conditions limits its long-term application. While there have been studies on its structural stability under heat and moisture, insight on the influence of light absorption is limited. We demonstrate that, under...

Operando Resonant Soft X-ray Scattering Studies of Chemical Environment and Interparticle Dynamics of Cu Nanocatalysts for CO2 Electroreduction

Yang Y
Roh I
Louisia S
Chen C
Jin J
Yu S
Salmeron M
Wang C
Yang P
2022

Understanding the chemical environment and interparticle dynamics of nanoparticle electrocatalysts under operating conditions offers valuable insights into tuning their activity and selectivity. This is particularly important to the design of Cu nanocatalysts for CO2 electroreduction due to their dynamic nature under bias. Here, we have developed operando electrochemical resonant soft X-ray scattering (EC-RSoXS) to probe the chemical identity of active sites during the dynamic structural transformation of Cu nanoparticle (NP) ensembles through 1...

Enhancing Biohybrid CO2 to Multicarbon Reduction via Adapted Whole-Cell Catalysts

Kim JM
Cestellos-Blanco S
Shen Y
Cai R
Yang P
2022

Catalytic CO2 conversion to renewable fuel is of utmost importance to establish a carbon-neutral society. Bioelectrochemical CO2 reduction, in which a solid cathode interfaces with CO2-reducing bacteria, represents a promising approach for renewable and sustainable fuel production. The rational design of biocatalysts in the biohybrid system is imperative to effectively reduce CO2 into valuable chemicals. Here, we introduce methanol adapted Sporomusa ovata (S....

Photosynthetic biohybrid coculture for tandem and tunable CO2 and N2 fixation

Cestellos-Blanco S
Chan RR
Shen Y
Kim JM
Tacken TA
Ledbetter R
Yu S
Seefeldt LC
Yang P
2022

Solar-driven bioelectrosynthesis represents a promising approach for converting abundant resources into value-added chemicals with renewable energy. Microorganisms powered by electrochemical reducing equivalents assimilate CO2, H2O, and N2 building blocks. However, products from autotrophic whole-cell biocatalysts are limited. Furthermore, biocatalysts tasked with N2 reduction are constrained by simultaneous energy-intensive autotrophy. To overcome these challenges, we designed a...

Supramolecular Assembly of Halide Perovskite Building Blocks

Zhu C
Jin J
Gao M
Oddo AM
Folgueras MC
Zhang Y
Lin C-K
Yang P
2022

The structural diversity and tunable optoelectronic properties of halide perovskites originate from the rich chemistry of the metal halide ionic octahedron [MX6]n− (M = Pb2+, Sb3+, Te4+, Sn4+, Pt4+, etc.; X = Cl–, Br–, and I–). The properties of the extended perovskite solids are dictated by the assembly, connectivity, and...

Nature of the Electrical Double Layer on Suspended Graphene Electrodes

Yang S
Zhao X
Lu Y-H
Barnard ES
Yang P
Baskin A
Lawson JW
Prendergast D
Salmeron M
2022

The structure of interfacial water near suspended graphene electrodes in contact with aqueous solutions of Na2SO4, NH4Cl, and (NH4)2SO4 has been studied using confocal Raman spectroscopy, sum frequency vibrational spectroscopy, and Kelvin probe force microscopy. SO42– anions were found to preferentially accumulate near the interface at an open circuit potential (OCP), creating an electrical...