Rationally designed Ru catalysts supported on TiN for highly efficient and stable hydrogen evolution in alkaline conditions DOI Creative Commons

Jia Zhao,

Ricardo Urrego‐Ortiz,

Nan Liao

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: July 29, 2024

Electrocatalysis holds the key to enhancing efficiency and cost-effectiveness of water splitting devices, thereby contributing advancement hydrogen as a clean, sustainable energy carrier. This study focuses on rational design Ru nanoparticle catalysts supported TiN (Ru NPs/TiN) for evolution reaction in alkaline conditions. The designed exhibit high mass activity 20 A mg−1Ru at an overpotential 63 mV long-term stability, surpassing present benchmarks commercial electrolyzers. Structural analysis highlights effective modification properties by substrate, while density functional theory calculations indicate strong adhesion particles substrates advantageous modulation adsorption energies via particle-support interactions. Finally, we assemble anion exchange membrane electrolyzer using NPs/TiN catalyst, which operates 5 cm−2 more than 1000 h with negligible degradation, exceeding performance requirements Our findings contribute efficient exploiting Designing stable electrocatalysts is great interest H2 fuel production. Here, authors catalyst TiN, achieving mg−1 conditions, operating over hours electrolyzer.

Language: Английский

Atomically dispersed materials: Ideal catalysts in atomic era DOI
Tao Gan, Dingsheng Wang

Nano Research, Journal Year: 2023, Volume and Issue: 17(1), P. 18 - 38

Published: May 25, 2023

Language: Английский

Citations

213
Electrocatalytic water splitting: Mechanism and electrocatalyst design DOI
Han Wu,

Qiaoxian Huang,

Yuanyuan Shi

et al.

Nano Research, Journal Year: 2023, Volume and Issue: 16(7), P. 9142 - 9157

Published: April 2, 2023

Language: Английский

Citations

175
Lattice Strain Engineering of Ni2P Enables Efficient Catalytic Hydrazine Oxidation‐Assisted Hydrogen Production DOI Open Access
Chao Feng,

Miaoyuan Lv,

Jiaxin Shao

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(42)

Published: July 11, 2023

Hydrazine-assisted water electrolysis provides new opportunities to enable energy-saving hydrogen production while solving the issue of hydrazine pollution. Here, synthesis compressively strained Ni2 P as a bifunctional electrocatalyst for boosting both anodic oxidation reaction (HzOR) and cathodic evolution (HER) is reported. Different from multistep synthetic method that induces lattice strain by creating core-shell structures, facile strategy developed tune via dual-cation co-doping. The obtained with compressive -3.62% exhibits significantly enhanced activity HzOR HER than counterparts tensile without strain. Consequently, optimized delivers current densities 10 100 mA cm-2 at small cell voltages 0.16 0.39 V hydrazine-assisted electrolysis, respectively. Density functional theory (DFT) calculations reveal promotes dissociation concurrently tunes adsorption strength intermediates, thereby facilitating process on P. As HzOR, reduces energy barrier potential-determining step dehydrogenation *N2 H4 H3 . Clearly, this work paves pathway lattice-strained electrocatalysts

Language: Английский

Citations

99
Fluorinated Ni‐O‐C Heterogeneous Catalyst for Efficient Urea‐Assisted Hydrogen Production DOI
Xuefei Xu, Habib Ullah, Muhammad Humayun

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(44)

Published: June 20, 2023

Abstract Constructing multiple heterogeneous structures allows for improving the electrocatalytic activity of NiO by incorporating active sites. Unfortunately, poor conductivity makes efficient charge transfer within difficult, thereby inhibiting improvement its intrinsic activity. Herein, F‐doped NiO/Ni@C catalyst (F‐NiO/Ni@C) is fabricated via a new organic‐inorganic hybrid approach, showing both advanced hydrogen evolution reaction (HER) and urea oxidation (UOR) The targeted F‐doping increases electron delocalization, facilitates from Ni to at nano‐interfaces. This interphase synergy provides ready‐to‐use F‐NiO sites, allowing F‐NiO/Ni@C achieve optimum H* adsorption Gibbs free energy HER lower barrier UOR. As result, as‐configured || cell requires an ultra‐low voltage 1.37 V 10 mA cm −2 in alkaline media (with 0.3 M urea), outperforming state‐of‐the‐art benchmark Pt/C|| RuO 2 (1.45 V). study reveals positive impact anion doping on useful guidelines designing monometallic catalysts UOR as well generation.

Language: Английский

Citations

81
Cooperative Ni(Co)‐Ru‐P Sites Activate Dehydrogenation for Hydrazine Oxidation Assisting Self‐powered H2 Production DOI
Yanmin Hu,

Tingting Chao,

Yapeng Li

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(35)

Published: July 10, 2023

Water electrolysis for H2 production is restricted by the sluggish oxygen evolution reaction (OER). Using thermodynamically more favorable hydrazine oxidation (HzOR) to replace OER has attracted ever-growing attention. Herein, we report a twisted NiCoP nanowire array immobilized with Ru single atoms (Ru1 -NiCoP) as superior bifunctional electrocatalyst toward both HzOR and hydrogen (HER), realizing an ultralow working potential of -60 mV overpotential 32 current density 10 mA cm-2 , respectively. Inspiringly, two-electrode electrolyzer based on overall splitting (OHzS) demonstrates outstanding activity record-high 522 at cell voltage 0.3 V. DFT calculations elucidate cooperative Ni(Co)-Ru-P sites in Ru1 -NiCoP optimize H* adsorption, enhance adsorption *N2 significantly lower energy barrier dehydrogenation. Moreover, self-powered system utilizing OHzS device driven direct fuel (DHzFC) achieve satisfactory rate 24.0 mol h-1 m-2 .

Language: Английский

Citations

72
Regulating Hydrogen/Oxygen Species Adsorption via Built‐in Electric Field ‐Driven Electron Transfer Behavior at the Heterointerface for Efficient Water Splitting DOI
Wenjie Zhang, Lei Yang, Zhi Li

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(16)

Published: Feb. 29, 2024

Abstract Alkaline water electrolysis (AWE) plays a crucial role in the realization of hydrogen economy. The design and development efficient stable bifunctional catalysts for both evolution reaction (HER) oxygen (OER) are pivotal to achieving high‐efficiency AWE. Herein, WC 1‐x /Mo 2 C nanoparticle‐embedded carbon nanofiber (WC C@CNF) with abundant interfaces is successfully designed synthesized. Benefiting from electron transfer behavior Mo , electrocatalysts C@CNF exhibit superior HER OER performance. Furthermore, when employed as anode cathode membrane electrode assembly devices, catalyst exhibits enhanced catalytic activity remarkable stability 100 hours at high current density 200 mA cm −2 towards overall splitting. experimental characterizations theoretical simulation reveal that modulation d‐band center C@CNF, achieved through asymmetric charge distribution resulting built‐in electric field induced by work function, enables optimization adsorption strength hydrogen/oxygen intermediates, thereby promoting kinetics This provides promising strategies designing highly active energy conversion fields.

Language: Английский

Citations

71
Ru/Ir‐Based Electrocatalysts for Oxygen Evolution Reaction in Acidic Conditions: From Mechanisms, Optimizations to Challenges DOI Creative Commons
Rong Qin, Guanzhen Chen,

Caihong Feng

et al.

Advanced Science, Journal Year: 2024, Volume and Issue: 11(21)

Published: March 19, 2024

Abstract The generation of green hydrogen by water splitting is identified as a key strategic energy technology, and proton exchange membrane electrolysis (PEMWE) one the desirable technologies for converting renewable sources into hydrogen. However, harsh anode environment PEMWE oxygen evolution reaction (OER) involving four‐electron transfer result in large overpotential, which limits overall efficiency production, thus efficient electrocatalysts are needed to overcome high overpotential slow kinetic process. In recent years, noble metal‐based (e.g., Ru/Ir‐based metal/oxide electrocatalysts) have received much attention due their unique catalytic properties, already become dominant acidic OER process applied commercial devices. these still face thorny problem conflicting performance cost. this review, first, metal briefly classified according forms existence, mechanisms outlined. Then, focus on summarizing improvement strategies with respect activity stability over years. Finally, challenges development prospects discussed.

Language: Английский

Citations

71
Interfacial Hydrogen Spillover on Pd-TiO2 with Oxygen Vacancies Promotes Formate Electrooxidation DOI
Zheng Tang, Yongjia Li,

Kaixin Zhang

et al.

ACS Energy Letters, Journal Year: 2023, Volume and Issue: 8(9), P. 3945 - 3954

Published: Aug. 28, 2023

Pd-based catalysts are crucial in direct formate fuel cells owing to their high stability and selectivity for the oxidation reaction (FOR) CO2, avoiding carbonaceous poisoning species (e.g., COad, CHx) alkaline media. However, kinetics of electrocatalysts considerably impeded by unfavorable adsorption hydrogen (Had), which serve as primary intermediators occlude active sites. Herein, we crafted electron-rich Pd nanoparticles on a TiO2 support with oxygen vacancies (Pd/Ov-TiO2) improve Had desorption. The as-prepared Pd/Ov-TiO2 exhibited mass activity 4.16 A mgPd–1, outperforming Pd/TiO2 without commercial Pd/C 1.41 2.72 times, respectively. Experimental characterizations density functional theory calculations revealed that oxygen-vacant can concurrently downshift d-band center facilitate spillover, thereby accelerating desorption FOR kinetics. Our findings provide strategy refine broader electrochemical uses.

Language: Английский

Citations

66
Microwave Quasi‐Solid State to Construct Strong Metal‐Support Interactions with Interfacial Electron‐Enriched Ru for Anion Exchange Membrane Electrolysis DOI
Pengfei Yang, Fusheng Liu,

Xingchao Zang

et al.

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 14(8)

Published: Dec. 28, 2023

Abstract Regulating the metal‐support interaction of anchored metal nanoclusters is recognized as valid approach to optimize electrocatalytic performance through tuning interfacial electronic structure. However, developing novel support and understanding electron accumulation on modulating reaction kinetics are still elusive. Herein, highly‐dispersed Ruthenium (Ru) onto phosphorous doped molybdenum boride (Ru/P‐MoB) developed ultrafast microwave‐plasma (60 s) approach. The synthesized Ru/P‐MoB impressively promote hydrogen evolution with low overpotentials 34, 45, 40 mV drive 10 mA cm −2 in alkaline freshwater, seawater acid media. Specially, it presents superior turnover frequency mass/specific activity relative Pt/C, Ru/C, Ru/MoB. Moreover, anion exchange membrane (AEM) electrolyzer cell based can achieve 500 1000 small voltages 1.71 1.78 V good durability. Experimental density functional theoretical (DFT) analysis reveal that strong interactions (Ru─Mo Ru─P bonds) generated electron‐enriched Ru, then favoring water‐molecule adsorption/dissociation optimal H intermediate adsorption free energy. This work provides designing avenue exploit electrocatalysts outstanding catalytic under high current at practical high‐temperature.

Language: Английский

Citations

66
Electrocatalytic nitrate-to-ammonia conversion on CoO/CuO nanoarrays using Zn–nitrate batteries DOI
Shanshan Chen, Gaocan Qi,

Ruilian Yin

et al.

Nanoscale, Journal Year: 2023, Volume and Issue: 15(48), P. 19577 - 19585

Published: Jan. 1, 2023

Zn-NO3- batteries can generate electricity while producing NH3 in an environmentally friendly manner, making them a very promising device. However, the conversion of NO3- to involves proton-assisted 8-electron (8e-) transfer process with high kinetic barrier, requiring high-performance catalysts realize potential applications this technology. Herein, we propose heterostructured CoO/CuO nanoarray electrocatalyst prepared on copper foam (CoO/CuO-NA/CF) that electrocatalytically and efficiently convert at low achieves maximum yield 296.9 μmol h-1 cm-2 Faraday efficiency (FE) 92.9% -0.2 V vs. reversible hydrogen electrode (RHE). Impressively, battery based monolithic CoO/CuO-NA/CF delivers 60.3 cm-2, FENH3 82.0%, power density 4.3 mW cm-2. This study provides paradigm for catalyst preparation energy-efficient production simultaneously generating electrical energy.

Language: Английский

Citations

64