Mediating Self‐Oxidation and Competitive Adsorption for Achieving High‐Selective Urea Oxidation Catalysis at Industrial‐Level Current Densities DOI Open Access
Pengfei Qiao, Guorui Li, Xiujuan Xu

et al.

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

Published: Dec. 23, 2024

Abstract Inhibiting the deactivation of nickel‐based catalysts caused by self‐oxidation and competitive adsorption behavior is still a major challenge for urea oxidation reaction (UOR), especially under industrial‐level current densities. In this study, crystalline NiSe 2 /amorphous NiFe‐LDH (NiSe /NiFe‐LDH) heterojunction catalyst rationally constructed selective electrocatalytic UOR. situ Raman spectra ex characterization results reveal that such structure can tailor impede accumulation NiOOH species during UOR process. Density function theory simulations disclose self‐driven charge transport from electron‐deficient region to electron‐rich would induce formation local electrophilic/nucleophilic adsorb electron‐donating ‐NH electron‐withdrawing C = O groups, respectively. This optimizes molecules hinders overaccumulation OH − ions on surface /NiFe‐LDH, which beneficial priority occurrence over oxygen evolution (OER) realization high selectivity. Benefiting tailored favorable adsorption, /NiFe‐LDH could act as high‐selective anode achieve ultrahigh 800 mAcm −2 only at 1.447 V. Besides, UV–vis spectrophotometry also unveiled has capability electrochemically degrade urea, offering great promise practical application potentials.

Language: Английский

Electrochemical Oxidation of Small Molecules for Energy‐Saving Hydrogen Production DOI
Hainan Sun, Xiaomin Xu, Liangshuang Fei

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(30)

Published: May 27, 2024

Abstract Electrochemical water splitting is a promising technique for the production of high‐purity hydrogen. Substituting slow anodic oxygen evolution reaction with an oxidation that thermodynamically more favorable enables energy‐efficient Moreover, this approach facilitates degradation environmental pollutants and synthesis value‐added chemicals through rational selection small molecules as substrates. Strategies small‐molecule electrocatalyst design are critical to electrocatalytic performance, focus on achieving high current density, selectivity, Faradaic efficiency, operational durability. This perspective discusses key factors required further advancement, including technoeconomic analysis, new reactor system design, meeting requirements industrial applications, bridging gap between fundamental research practical product detection separation. aims advance development hybrid electrolysis applications.

Language: Английский

Citations

41
Mott–Schottky Barrier Enabling High‐Performance Hydrazine‐Assisted Hydrogen Generation at Ampere‐Level Current Densities DOI

Yaping Huang,

Xia Zhang, Linfeng Li

et al.

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

Published: April 18, 2024

Abstract Local electron density manipulation can optimize the adsorption and desorption nature of catalysts leading to enhanced catalytic activity for water oxidation. Construction a Mott–Schottky barrier allows transition in because their different Fermi levels. Herein, Pt@NiFc‐MOF heterojunction is constructed, which electrons are transferred from NiFc‐MOF Pt as triggered by formed built‐in electric field at interface. The as‐prepared reveals exceptional performance toward hydrazine oxidation reaction (HzOR), hydrogen evolution (HER), overall splitting (OHzS) ampere‐level current densities. advanced configured also be further evidenced concept direct liquid N 2 H 4 /H O fuel cell (Pt@NiFc‐MOF//Pt Net), yielding maximum power 415.2 mW cm ‒2 80°C work stably 190 h 500 mA (at 25°C). One more function clarified well, that it purify hydrazine‐rich wastewater 718 6 ppb (less than U.S. Environmental Protection Agency 10 ppb) 120 min . This represents breakthrough interface engineering metal–organic frameworks (MOFs) industry‐level generation its beyond.

Language: Английский

Citations

34
Highly selective urea electrooxidation coupled with efficient hydrogen evolution DOI Creative Commons
Guangming Zhan,

Lufa Hu,

Hao Li

et al.

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

Published: July 14, 2024

Abstract Electrochemical urea oxidation offers a sustainable avenue for H 2 production and wastewater denitrification within the water-energy nexus; however, its wide application is limited by detrimental cyanate or nitrite instead of innocuous N . Herein we demonstrate that atomically isolated asymmetric Ni–O–Ti sites on Ti foam anode achieve selectivity 99%, surpassing connected symmetric Ni–O–Ni counterparts in documented Ni-based electrocatalysts with below 55%, also deliver evolution rate 22.0 mL h –1 when coupled to Pt counter cathode under 213 mA cm –2 at 1.40 V RHE These sites, featuring oxygenophilic adjacent Ni, favor interaction carbonyl over amino groups urea, thus preventing premature resonant C⎓N bond breakage before intramolecular N–N coupling towards evolution. A prototype device powered commercial Si photovoltaic cell further developed solar-powered on-site urine processing decentralized production.

Language: Английский

Citations

29
Water-Stable Pillared Three-Dimensional Zn–V Bimetal–Organic Framework for Promoted Electrocatalytic Urea Oxidation DOI
Reza Abazari,

Soheila Sanati,

Paweł Stelmachowski

et al.

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: 63(12), P. 5642 - 5651

Published: March 12, 2024

Urea oxidation reaction (UOR) is one of the potential routes in which urea-rich wastewater used as a source energy for hydrogen production. Metal–organic frameworks (MOFs) have promising applications electrocatalytic processes, although there are still challenges identifying MOFs' molecular regulation and obtaining practical catalytic systems. The current study sought to synthesize [Zn6(IDC)4(OH)2(Hprz)2]n (Zn-MOF) with three symmetrically independent Zn(II) cations connected via linear N-donor piperazine (Hprz), rigid planar imidazole-4,5-dicarboxylate (IDC3–), −OH ligands, revealing 3,4T1 topology. optimized noble-metal-free Zn0.33V0.66-MOF/NF electrocatalysts show higher robustness performance compared those parent Zn monometallic MOF/NF electrode other bimetallic MOFs different Zn–V molar ratios. low 1.42 V (vs RHE) at 50 mA cm–2 1.0 M KOH 0.33 urea required by developed Zn0.33V0.66-MOF makes its application UOR more feasible. availability exposed active sites, ion diffusion path, conductivity result from distinctive configuration synthesized electrocatalyst, highly stable capable synergistic effects, consequently enhancing desired reaction. research contributes introducing practical, cost-effective, sustainable solution decompose produce hydrogen.

Language: Английский

Citations

24
Sulfurization-induced lattice disordering in high-entropy catalyst for promoted bifunctional electro-oxidation behavior DOI
Jing Chen, Kexin Wang,

Zimeng Liu

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 489, P. 151234 - 151234

Published: April 15, 2024

Language: Английский

Citations

11
Multi-metallic electrocatalysts as emerging class of materials: opportunities and challenges in the synthesis, characterization, and applications DOI
Muhammad Israr, Muhammad Humayun, Munzir H. Suliman

et al.

Catalysis Reviews, Journal Year: 2024, Volume and Issue: unknown, P. 1 - 61

Published: May 28, 2024

Nowadays, extensive efforts have been devoted to the fabrication and design of metalbased catalysts with high activity, selectivity, stability. Theoretical experimental investigations empowered construction a variety techniques tune catalytic efficiency by monitoring their size, morphology, composition, crystal structure. Multimetal (MMCs) provide revolutionary synergistic effect between metals, which is promising strategy enhance catalysts' productivity product selectivity. The purpose this article familiarize readers most uptodate information regarding synthesis classification MMCs. key roles MMCs electrocatalysts in applications such as CO2 conversion via electrochemical reduction reaction (ECO2RR), H2 evolution (HER), O2 (OER), (ORR), N2 (NRR), methanol oxidation (MOR), ethanol (EOR), formic acid (FAOR), urea (UOR) are summarized. This review also addressed challenges prospects for multimetallic catalyst design, characterization, applications. will clear roadmap research progress electrocatalytic

Language: Английский

Citations

10
Efficient urea removal with hydroperoxide production in bipolar membrane electrochemical cell using MoNiOOH nanoarray anode electrocatalyst DOI
Xin Li,

Shuyue Ma,

Lingli Tu

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125158 - 125158

Published: Feb. 1, 2025

Language: Английский

Citations

1
Interface engineering of Ni3S2@NiFe-LDH core-shell heterostructure to achieve energy-saving hydrogen production DOI
Yun Chen,

Yuewen Wu,

Mingpeng Chen

et al.

Journal of Alloys and Compounds, Journal Year: 2024, Volume and Issue: unknown, P. 177855 - 177855

Published: Nov. 1, 2024

Language: Английский

Citations

6
Triphenylamine-Substituted Ni(II) Porphyrins for Urea Electro-oxidation DOI
Shun Lu, Xingqun Zheng, Yi Zeng

et al.

Inorganic Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 23, 2024

Porphyrin-based molecular catalysts possess a typical aromatic macrocyclic structure regarding their metal centers and coordination frameworks, allowing for the development of promising electrocatalysts through precise selection porphyrin ligand. However, reports on metalloporphyrins as electrocatalytic urea oxidation reaction (UOR) remain scarce. With these considerations in mind, triphenylamine-Ni(II) (NiPor-TPA) was synthesized solvothermal approach from 5,10,15,20-tetrakis [4-(diphenylamino)phenyl]porphyrin nickel(II) acetate this work. Experimental results reveal that introduction Ni species can serve active sites activate efficiently, thus prepared deliver better activity than metal-free TPA. The NiPor-TPA electrode delivers lowest potential 1.34 V versus reversible hydrogen (RHE) at 10 mA cm

Language: Английский

Citations

5
Double Hydroxide Nanocatalysts for Urea Electrooxidation Engineered toward Environmentally Benign Products DOI Creative Commons
Yuwei Yang, Jodie A. Yuwono, Todd N. Whittaker

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(35)

Published: July 14, 2024

Recent advancements in the electrochemical urea oxidation reaction (UOR) present promising avenues for wastewater remediation and energy recovery. Despite progress toward optimized efficiency, hurdles persist steering products away from environmentally unfriendly products, mostly due to a lack of understanding structure-selectivity relationships. In this study, UOR performance Ni Cu double hydroxides, which show marked differences their reactivity selectivity is evaluated. CuCo hydroxides predominantly produce N

Language: Английский

Citations

4