Tailored Electronic Structure of Ir in High Entropy Alloy for Highly Active and Durable Bifunctional Electrocatalyst for Water Splitting under an Acidic Environment

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(26)

Published: March 27, 2023

Proton-exchange-membrane water electrolysis (PEMWE) requires an efficient and durable bifunctional electrocatalyst for the hydrogen evolution reaction (HER) oxygen (OER). Herein, Ir-based is designed using high entropy alloy (HEA) platform of ZnNiCoIrX with two elements (X: Fe Mn). A facile dealloying in vacuum system enables construction a nanoporous structure crystallinity Zn as sacrificial element. Especially, Mn incorporation into HEAs tailors electronic Ir site, resulting d-band center being far away from Fermi level. Downshifting weakens adsorption energy intermediates, which beneficial catalytic reactions. Despite low content, ZnNiCoIrMn delivers only 50 mV overpotential HER at -50 mA cm-2 237 OER 10 . Furthermore, shows almost constant voltage 100 h stability number 3.4 × 105 nhydrogen nIr-1 2.4 noxygen , demonstrating exceptional durability HEA platform. The compositional engineering limits diffusion by effects simultaneously active sites, modified cohesive energies, all can suppress dissolution elements.

Language: Английский

---

Bifunctional PdPt bimetallenes for formate oxidation‐boosted water electrolysis

Carbon Energy, Journal Year: 2023, Volume and Issue: 5(12)

Published: April 4, 2023

Abstract Small‐molecule electrooxidation‐boosted water electrolysis (WE) is an energy‐saving method for hydrogen (H 2 ) production. Herein, PdPt bimetallenes (PdPt BMLs) are obtained through the simple galvanic replacement reaction. BMLs reveal 2.93‐fold enhancement in intrinsic electroactivity and 4.53‐fold mass formate oxidation reaction (FOR) with respect to Pd metallenes (Pd MLs) at 0.50 V potential due synergistic effect. Meanwhile, introduction of Pt atoms also considerably increases evolution (HER) MLs alkaline medium, which even exceeds that use commercial nanocrystals. Inspired by outstanding FOR HER bifunctional BMLs, a two‐electrode FOR‐boosted WE system (FOR‐WE) constructed using as cathode anode. The FOR‐WE only requires operational voltage 0.31 achieve H production, 1.48 lower than (ca. 1.79 V) traditional system.

Language: Английский

---

Ir Nanoparticles Anchored on Metal‐Organic Frameworks for Efficient Overall Water Splitting under pH‐Universal Conditions

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(17)

Published: March 2, 2023

The construction of high-activity and low-cost electrocatalysts is critical for efficient hydrogen production by water electrolysis. Herein, we developed an advanced electrocatalyst anchoring well-dispersed Ir nanoparticles on nickel metal-organic framework (MOF) Ni-NDC (NDC: 2,6-naphthalenedicarboxylic) nanosheets. Benefiting from the strong synergy between MOF through interfacial Ni-O-Ir bonds, synthesized Ir@Ni-NDC showed exceptional electrocatalytic performance evolution reaction (HER), oxygen (OER) overall splitting in a wide pH range, superior to commercial benchmarks most reported electrocatalysts. Theoretical calculations revealed that charge redistribution bridge induced optimization H2 O, OH* H* adsorption, thus leading accelerated electrochemical kinetics HER OER. This work provides new clue exploit bifunctional pH-universal splitting.

Language: Английский

---

In Situ Reconstruction of Partially Hydroxylated Porous Rh Metallene for Ethylene Glycol‐Assisted Seawater Splitting

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 32(31)

Published: May 17, 2022

Abstract Designing efficient and durable electrocatalysts for seawater electrolysis shows a great research prospect, but it remains significant challenge. Herein, we report the partially hydroxylated Rh metallene (Rh/RhOOH metallene) with porous, ultrathin, defect‐rich hetero‐phase structure ethylene glycol (EG)‐assisted electrolysis. In parallel, unique redox effect of RhOOH species EG as well electroreduction riggers in situ reconstruction catalyst during electrocatalysis, which further produces active to optimize catalytic activity center surface reaction. Benefiting from Rh/RhOOH heterogeneous structure, exhibits superior electrocatalytic performance towards hydrogen evolution reaction (HER, overpotential 29 mV) oxidation (EGOR, specific 1.051 mA cm –2 ). Encouragingly, constructed EG‐assisted system, only needs low cell voltage 0.678 V achieve current density 10 energy‐saving H 2 production, significantly reduces energy consumption compared conventional

Language: Английский

---

Interfacial engineering of holey platinum nanotubes for formic acid electrooxidation boosted water splitting

Journal of Energy Chemistry, Journal Year: 2022, Volume and Issue: 77, P. 209 - 216

Published: Oct. 20, 2022

Language: Английский

---

Activating Amorphous Ru Metallenes Through Co Integration for Enhanced Water Electrolysis

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(28)

Published: June 11, 2023

Abstract Designing efficient bifunctional electrocatalysts with excellent activity and robust stability presents a central challenge for the large‐scale commercialization of water electrolysis. Herein, facile approach is reported construct atomically thin amorphous RuM (MCo, Fe, or Ni) bimetallenes as high‐performance toward both electrochemical hydrogen evolution reaction (HER) oxygen (OER). The RuCo bimetallene manifests characterized by low required overpotentials, superior price activity, durability well cell potential splitting performance, outperforming Pt/C RuO 2 benchmark catalysts. Combined operando X‐ray absorption spectroscopy investigation theoretical simulations reveal synergism taking place between binary constituents, in which Co serves promotive role along HER/OER pathway, contributing via optimal binding to *OH dissociation modulating Ru electronic structure favorably, hence rendering high catalytic centers alkaline HER OER.

Language: Английский

---

AuCu nanofibers for electrosynthesis of urea from carbon dioxide and nitrite

Cell Reports Physical Science, Journal Year: 2022, Volume and Issue: 3(5), P. 100869 - 100869

Published: April 25, 2022

Carbon dioxide reduction reaction (CO2RR) is a promising technology for mitigating greenhouse gas emission and achieving carbon neutrality. However, coupling CO2RR with other reactions to produce high value-added chemicals remains challenge. In this work, we report self-assembled nanofibers composed of ultrathin AuCu alloy nanowires possessing Boerdijk-Coxeter structure (111)-dominant facets the electrosynthesis urea by nitrite (NO2−RR). The rich structural defects bimetallic composition provide large number highly catalytically active sites. constructed display excellent synthesis performance in electrolyte solution containing 0.01 M KNO2 continuous drumming CO2, yield rate up 3,889.6 μg h−1 mg−1cat. faradic efficiency 24.7% at −1.55 V (versus Ag/AgCl). This work provides feasible method rational design under ambient conditions.

Language: Английский

---

Nanoarchitectonics of Metallene Materials for Electrocatalysis

ACS Nano, Journal Year: 2023, Volume and Issue: 17(14), P. 13017 - 13043

Published: June 27, 2023

Controlling the synthesis of metal nanostructures is one approach for catalyst engineering and performance optimization in electrocatalysis. As an emerging class unconventional electrocatalysts, two-dimensional (2D) metallene electrocatalysts with ultrathin sheet-like morphology have gained ever-growing attention exhibited superior electrocatalysis owing to their distinctive properties originating from structural anisotropy, rich surface chemistry, efficient mass diffusion capability. Many significant advances synthetic methods electrocatalytic applications 2D metallenes been obtained recent years. Therefore, in-depth review summarizing progress developing electrochemical highly needed. Unlike most reported reviews on metallenes, this starts by introducing preparation based classification metals (e.g., noble metals, non-noble metals) instead methods. Some typical strategies preparing each kind are enumerated detail. Then, utilization applications, especially conversion reactions, including hydrogen evolution reaction, oxygen reduction fuel oxidation CO2 N2 comprehensively discussed. Finally, current challenges opportunities future research energy proposed.

Language: Английский

---

Oxygen-Bridged Stabilization of Single Atomic W on Rh Metallenes for Robust and Efficient pH-Universal Hydrogen Evolution

ACS Nano, Journal Year: 2023, Volume and Issue: 17(11), P. 10733 - 10747

Published: May 17, 2023

Highly efficient and durable electrocatalysts are of the utmost importance for sustainable generation clean hydrogen by water electrolysis. Here, we present a report an atomically thin rhodium metallene incorporated with oxygen-bridged single atomic tungsten (Rh-O-W) as high-performance electrocatalyst pH-universal evolution reaction. The Rh-O-W delivers ascendant electrocatalytic HER performance, characterized exceptionally low overpotentials, ultrahigh mass activities, excellent turnover frequencies, robust stability negligible deactivation, in electrolytes, outperforming that benchmark Pt/C, Rh/C numerous other reported precious-metal catalysts. Interestingly, promoting feature -O-W sites is understood via operando X-ray absorption spectroscopy characterization theoretical calculations. On account electron transfer equilibration processes take place between binary components metallenes, fine-tuning density states localization at Rh active attained, hence near-optimal adsorption.

Language: Английский

---

Mesoporous PtPb Nanosheets as Efficient Electrocatalysts for Hydrogen Evolution and Ethanol Oxidation

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(30)

Published: May 26, 2023

Using a one-pot hydrothermal method with ethylenediamine, we have synthesized mesoporous PtPb nanosheets that exhibit exceptional activity in both hydrogen evolution and ethanol oxidation. The resulting Pt-enriched structure up to 80 % atomic content of Pt. synthetic generated significant structure, formed through the dissolution Pb species. These advanced structures enable achieve current density 10 mA cm-2 an extreme low overpotential 21 mV for under alkaline conditions. Furthermore, superior catalytic stability highest is 5.66 times higher than commercial Pt/C. This research opens new possibilities designing mesoporous, two-dimensional noble-metal-based materials electrochemical energy conversion excellent performance.

Language: Английский

---