Well‐defined nanostructures of high entropy alloys for electrocatalysis DOI Creative Commons
Jie Chen, Liping Ren, Xin Chen

et al.

Exploration, Journal Year: 2024, Volume and Issue: unknown

Published: July 2, 2024

High-entropy alloys (HEAs) have attracted significant attention for electrocatalytic energy conversion by virtue of their promisingly high efficiency, stability, and low cost. Recently, encouraging progress has been made in tuning the structure composition HEAs used electrolyzers fuel cells. However, understanding on synthetic methods structure-property-performance relationship well-defined nanostructures is still inadequate. To gain insight into future research directions electrocatalysis, this paper, commonly to obtain (0D nanoparticles, 1D nanowires, 2D nanosheets/nanoplates, 3D nanoporous structures, other three-dimensional morphologies) are first summarized. Then, authors discuss application several typical reactions, including hydrogen evolution reaction, oxygen reduction alcohol oxidation carbon dioxide nitrogen formic acid reaction. Finally, a practical perspective nanostructured electrocatalysts provided.

Language: Английский

Intermetallic Single-Atom Alloy In–Pd Bimetallene for Neutral Electrosynthesis of Ammonia from Nitrate DOI
Minghao Xie, Sishuang Tang, Li Zhao

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(25), P. 13957 - 13967

Published: June 19, 2023

Harvesting recyclable ammonia (NH3) from the electrocatalytic reduction of nitrate (NO3RR) offers a sustainable strategy to close ecological nitrogen cycle nitration contamination in an energy-efficient and environmentally friendly manner. The emerging intermetallic single-atom alloys (ISAAs) are recognized achieve highest site density single atoms by isolating contiguous metal into sites stabilized another within structure, which holds promise couple catalytic benefits nanocrystals catalysts for promoting NO3RR. Herein, ISAA In-Pd bimetallene, Pd isolated surrounding In atoms, is reported boost neutral NO3RR with NH3 Faradaic efficiency (FE) 87.2%, yield rate 28.06 mg h-1 mgPd-1, exceptional stability increased activity/selectivity over 100 h 20 cycles. structure induces substantially diminished overlap d-orbitals narrowed p-d hybridization In-p Pd-d states around Fermi level, resulting stronger NO3- adsorption depressed energy barrier potential-determining step Further integrating catalyst Zn-NO3- flow battery as cathode delivers power 12.64 mW cm-2 FE 93.4% production.

Language: Английский

Citations

178

Spatially Confined PdHx Metallenes by Tensile Strained Atomic Ru Layers for Efficient Hydrogen Evolution DOI
Jinchang Fan, Zhipeng Feng,

Yajing Mu

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(10), P. 5710 - 5717

Published: March 6, 2023

Hydride metallenes show great potential for hydrogen-related catalytic applications due to favorable electronic structures modulated by interstitial hydrogen atoms and large active surface areas of metallenes. Metallene nanostructures generally have compressive strain relative bulk, which can affect both the stability behavior hydride but in general cannot be controlled. Here, we demonstrate highly stable PdHx with a tensile strained Ru layer reveal spatial confinement effect skin multiple spectroscopic characterizations molecular dynamics simulations. These PdHx@Ru 4.5% expanded outer exhibit outstanding alkaline evolution reaction activity low overpotential 30 mV at 10 mA cm-2 robust negligible decay after 10,000 cycles, are superior commercial Pt/C most reported Ru-based electrocatalysts. Control experiments first-principles calculations that lowers energy barrier H2O dissociation provides moderate adsorption energy.

Language: Английский

Citations

107

Multisite Synergism‐Induced Electron Regulation of High‐Entropy Alloy Metallene for Boosting Alkaline Hydrogen Evolution Reaction DOI

Qiqi Mao,

Mu Xu,

Kai Deng

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(42)

Published: June 14, 2023

Abstract Designing the high‐entropy alloys (HEAs) electrocatalysts with controllable nanostructures is of great significance for development efficient alkaline hydrogen evolution reaction (HER) electrocatalysts. In this study, an ultrathin HEA‐PdPtRhIrCu metallene abundant lattice distortions and defects prepared via a facile one‐step hydrothermal method. The synthesized exhibits superior HER performance in 1 m KOH solution, where required overpotential only 15 mV to reach current density −10 mA cm −2 while possessing low Tafel slope 37 dec −1 . Density functional theory calculations further prove that synergistic effect five elements can optimize electronic structure enhance activity catalysts. particular, strong coupling bonding arising from interaction between multi‐metal components facilitate electron transfer surface high electroactivity. Moreover, optimized Pt promotes optimal PtH binding at site, thus promoting performance.

Language: Английский

Citations

68

Electrochemical Co-Production of Ammonia and Biodegradable Polymer Monomer Glycolic Acid via the Co-Electrolysis of Nitrate Wastewater and Waste Plastic DOI

Tianlun Ren,

Zhongyao Duan,

Huizhen Wang

et al.

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(15), P. 10394 - 10404

Published: July 25, 2023

Electrochemical reformation of nitrate wastewater and poly(ethylene terephthalate) (PET) plastic waste into ammonia (NH3) fine chemicals is a sustainable strategy for resource utilization. Herein, co-production system glycolic acid (GA, degradable polymer monomer) constructed by coupling reduction ethylene glycol (EG, in PET hydrolysate) oxidation. Low-crystalline CoOOH (LC-CoOOH/CF) Pd nanothorns (Pd NTs/NF) grown situ on the metal foam substrates are employed as cathode anode, respectively. The high density amorphous regions LC-CoOOH/CF enables enhanced adsorption provides abundant active sites, ultimately leading to an Faradic efficiency (FE) 97.38 ± 1.0% at −0.25 V vs reversible hydrogen electrode (RHE). Meanwhile, unique nanothorn morphology endows NTs/NF with high-curvature tip, triggering tip effect (TE) promote highly selective oxidation EG GA. Furthermore, two-electrode system, NH3 GA operated low energy consumption (onset voltage: 0.5 V), much lower than traditional electrolysis process (1.4 V). This study method utilization co-produce value-added chemicals.

Language: Английский

Citations

60

High Entropy‐Driven Role of Oxygen Vacancies for Water Oxidation DOI
Yifan Liu, Caichao Ye, Long Chen

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(25)

Published: Jan. 30, 2024

Abstract Oxygen vacancy engineering is a promising strategy to enhance the electrocatalytic activities in conventional metal oxide electrocatalysts. However, utilization of oxygen vacancies high‐entropy oxides remains unknown, primarily due challenges associated with facile introduction and explanation their roles complex systems. Herein, into realized unique high entropy‐driven role for evolution reaction (OER) process revealed. A low‐temperature surface carbonization–decarbonization approach developed introduce regulate spinel (HEOs). The HEOs can both facilitate pre‐oxidation faster OH − adsorption induce bridge site pathway easier deprotonation, distinctive where favor * yet hinder deprotonation. Consequently, as‐prepared (HEOs‐Ov) exhibit superior OER activities, outperforming most reported oxide‐based Besides, this universal method be extended other different configuration entropies scaled up. work paves way exploration toward electrocatalysis fields.

Language: Английский

Citations

55

Interfacial built‐in electric fields facilitating surface reconstruction in heterojunction electrocatalysts for boosting water oxidation and simulated seawater oxidation DOI
Hui Xu, Lei Jin, Kun Wang

et al.

Fuel, Journal Year: 2024, Volume and Issue: 369, P. 131716 - 131716

Published: April 17, 2024

Language: Английский

Citations

40

Optimizing Intermediate Adsorption over PdM (M=Fe, Co, Ni, Cu) Bimetallene for Boosted Nitrate Electroreduction to Ammonia DOI
Yuanbo Zhou, Lifang Zhang, Zebin Zhu

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(18)

Published: March 7, 2024

Electrochemical reduction of nitrate to ammonia (NO

Language: Английский

Citations

37

Interstitial Boron Atoms in Pd Aerogel Selectively Switch the Pathway for Glycolic Acid Synthesis from Waste Plastics DOI Open Access
Junliang Chen, Miaomiao Jiang, Fangzhou Zhang

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: July 28, 2024

Abstract Electro‐reforming of poly(ethylene terephthalate) (PET) into valuable chemicals is garnering significant attention as it opens a mild avenue for waste resource utilization. However, achieving high activity and selectivity C2 products during ethylene glycol (EG) oxidation in PET hydrolysate on Pd electrocatalysts remains challenging. The strong interaction between carbonyl (*CO) intermediates leads to undesirable over‐oxidation poisoning sites, which hinders the highly efficient production. Herein, nonmetallic alloying strategy employed fabricate Pd‐boron alloy aerogel (PdB), wherein B atoms are induced regulate electron structure surface oxophilicity. This approach allows remarkable mass 6.71 A mg −1 , glycolic acid (GA) Faradaic efficiency (FE) 93.8%, stable 100 h cyclic electrolysis. In situ experiments density functional theory calculations reveal contributions inserted lattice effective EG‐to‐GA conversion. Interestingly, heightened oxophilicity regulated electronic by incorporation weakened *CO adsorption enhanced hydroxyl species affinity accelerate oxidative *OH adspecies formation, thereby synergistically avoiding boosting GA synthesis. work provides insights rational design high‐performance synthesis via an oxophilic motifs strategy.

Language: Английский

Citations

31

Recent progress in two-dimensional metallenes and their potential application as electrocatalyst DOI
Umer Shahzad, Mohsin Saeed, Muhammad Fazle Rabbee

et al.

Journal of Energy Chemistry, Journal Year: 2024, Volume and Issue: 94, P. 577 - 598

Published: March 16, 2024

Language: Английский

Citations

24

Support engineering modulated Pt/hierarchical MoSe2@mesoporous hollow carbon spheres for efficient methanol-assisted water splitting DOI
Fulin Yang, Wei Qiao,

Lice Yu

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 483, P. 149055 - 149055

Published: Jan. 26, 2024

Language: Английский

Citations

23