Regulating Reconstruction‐Engineered Active Sites for Accelerated Electrocatalytic Conversion of Urea

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(36)

Published: June 14, 2024

Reconstruction-engineered electrocatalysts with enriched high active Ni species for urea oxidation reaction (UOR) have recently become promising candidates energy conversion. However, to inhibit the over-oxidation of brought by valence state Ni, tremendous efforts are devoted obtaining low-value products nitrogen gas avoid toxic nitrite formation, undesirably causing inefficient utilization cycle. Herein, we proposed a mediation engineering strategy significantly boost high-value formation help close loop employment economy. Specifically, platinum-loaded nickel phosphides (Pt-Ni

Language: Английский

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Manipulating d‐Band Center of Ru Sites in Branched RuO₂ Nanofibers Enables Significantly Enhanced Alkaline Overall Water Splitting Performance

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

Published: Oct. 9, 2024

Abstract Although ruthenium dioxide (RuO 2 ) is an efficacious oxygen evolution reaction (OER) catalyst in acidic media, its performance alkaline conditions subpar and it also ineffective for hydrogen (HER) common electrolytes. Here, effective phosphorus (P)‐doping strategy introduced to manipulate the d ‐band center of (Ru) sites, attenuating adsorption energy HER intermediates lowering barrier OER, thereby significantly accelerating both OER performance. The representative 10%P‐RuO nanofibers (NFs) presents ultralow overpotential 177.9 mV at 1 A cm −2 long‐term stability 300 h m KOH toward HER, greatly exceeding those benchmark platinum (Pt)/C catalyst. Moreover, NFs exhibits exceptional with a low 250 10 mA (η desirable 150 , which far better than commercial RuO many other typical previously reported catalysts. Additionally, overall water electrolytic cell using as anode cathode necessitates working voltage 1.52 V demonstrates over 100 outperforming electrolysis cells.

Language: Английский

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Hollow Mo/MoS_Vn Nanoreactors with Tunable Built‐in Electric Fields for Sustainable Hydrogen Production

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

Published: Dec. 8, 2024

Abstract Constructing built‐in electric field (BIEF) in heterojunction catalyst is an effective way to optimize adsorption/desorption of reaction intermediates, while its precise tailor achieve efficient bifunctional electrocatalysis remains great challenge. Herein, the hollow Mo/MoS Vn nanoreactors with tunable BIEFs are elaborately prepared simultaneously promote hydrogen evolution (HER) and urea oxidation (UOR) for sustainable production. The BIEF induced by sulfur vacancies can be modulated from 0.79 0.57 0.42 mV nm −1 , exhibits a parabola‐shaped relationship HER UOR activities, V1 nanoreactor moderate presents best activity. Theoretical calculations reveal that evidently facilitate breakage N─H bond UOR. electrolyzer assembled delivers cell voltage 1.49 V at 100 mA cm −2 which 437 lower than traditional water electrolysis, also excellent durability 200 h. Life cycle assessment indicates HER||UOR system possesses notable superiority across various environment impact energy consumption. This work provide theoretical experimental direction on rational design advanced materials energy‐saving eco‐friendly

Language: Английский

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Boosting Urea-Assisted Natural Seawater Electrolysis in 3D Leaf-Like Metal–Organic Framework Nanosheet Arrays Using Metal Node Engineering

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(22), P. 28625 - 28637

Published: May 20, 2024

Metal node engineering, which can optimize the electronic structure and modulate composition of poor electrically conductive metal–organic frameworks, is great interest for electrochemical natural seawater splitting. However, mechanism underlying influence mixed-metal nodes on electrocatalytic activities still ambiguous. Herein, a strategic design comprehensively demonstrated in mixed Ni Co metal redox-active centers are uniformly distributed within NH2–Fe-MIL-101 to obtain synergistic effect overall enhancement activities. Three-dimensional metallic MOF nanosheet arrays, consisting three different nodes, were situ grown foam as highly active stable bifunctional catalyst urea-assisted A well-defined NH2–NiCoFe-MIL-101 reaches 1.5 cm–2 at 360 mV oxygen evolution reaction (OER) 0.6 295 hydrogen (HER) freshwater, substantially higher than its bimetallic monometallic counterparts. Moreover, electrode exhibits eminent catalytic activity stability seawater-based electrolytes. Impressively, two-electrode alkaline electrolysis cell based needs only 1.56 yield 100 mA cm–2, much lower 1.78 V cells superior long-term current density 80 h.

Language: Английский

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Synthesis of polymetallic oxide nanoarrays as efficient hydrogen evolution reaction electrocatalyst for alkaline seawater and urea splitting

Fuel, Journal Year: 2024, Volume and Issue: 372, P. 132281 - 132281

Published: June 21, 2024

Language: Английский

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Local Charge Modulation Induced the Formation of High‐Valent Nickel Sites for Enhanced Urea Electrolysis

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(41)

Published: Aug. 17, 2024

Abstract Ni‐based electrocatalysts are considered to be significantly promising candidates for electrocatalytic urea oxidation reaction (UOR). However, their UOR activity and stability severely enslaved by the inevitable Ni group self‐oxidation phenomenon. In this study, glassy state NiFe LDH with uniform Cu dopant (Cu‐NiFe LDH) a simple sol–gel strategy is successfully synthesized. When served as catalyst, Cu‐NiFe required 123 mV lower potential at both 10 100 mA cm −2 in comparison conventional anodic OER. It can also operate steadily more than 300 h . The in‐depth investigation reveals that incorporation optimize local electronic structure of species induce high‐valent sites. sites would act active center during proposed energetically favorable route, which directly reacts on without inducing formation NiOOH species, resulting boosted stability.

Language: Английский

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Electronic engineering induced ultrafine non-noble nanoparticles for high-performance hydrogen evolution from ammonia borane hydrolysis

Fuel, Journal Year: 2024, Volume and Issue: 381, P. 133424 - 133424

Published: Oct. 17, 2024

Language: Английский

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Crystalline Ru-Decorated MOF-Derived Amorphous CoMo-LDH Nanosheet Arrays as Bifunctional Catalysts for Overall Natural Seawater Electrolysis

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 24, 2024

The construction of an amorphous/crystalline heterostructure MOF-derived electrocatalysts offers intriguing pathway to improve hydrogen production efficiency, but it has received little attention. Here, we report crystalline Ru-decorated amorphous CoMo-LDH nanosheet arrays as highly active and robust bifunctional for natural seawater electrolysis. Benefiting from the abundant interfaces, Ru-CoMo-LDH catalyst exhibits excellent activity toward OER under fresh seawater, in particular; requires only 257 406 mV overpotential at 10 500 mA cm

Language: Английский

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Self‐Encapsulated Ni Nanoparticles on Delignified Wood Carbon for Efficient Urea‐Assisted Hydrogen Production

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

Published: Oct. 8, 2024

Abstract Developing efficient, low‐cost electrocatalysts for industrial‐level hydrogen production remains a significant challenge. Here lattice‐distorted Ni nanoparticles (NPs) encapsulated within nitrogen‐doped carbon shell on delignified wood (Ni‐NC@DWC) are constructed through chitosan‐induced assembly and the pyrolysis process. Experimental theoretical results indicate that lattice distortion due to strong metal‐support interactions, boosts electron transfer reaction intermediate adsorption/desorption, enhancing both urea oxidation (UOR) evolution (HER). Interestingly, active center 3+ ‐O is dynamically cyclically generated during UOR. When utilized as self‐standing electrode in an alkaline electrolyte, Ni‐NC@DWC exhibits low potentials of 24 mV 1.244 V at 100 mA cm −2 HER UOR, respectively. Moreover, achieves ultrasmall cell voltage 1.13 urea‐assisted water splitting can operate stably over 1000 h. Furthermore, when it self‐assembled anion exchange membrane (AEM) electrolyzer, requires only 1.62 2000 industrial operates 150 h without degradation, confirming highly attractive economical, sustainable, scalable production.

Language: Английский

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Twin-distortion modulated ultra-low coordination PtRuNi-Ox catalyst for enhanced hydrogen production from chemical wastewater

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

Published: Nov. 22, 2024

The development of efficient and robust catalysts for hydrogen evolution reaction is crucial advancing the economy. In this study, we demonstrate that ultra-low coordinated hollow PtRuNi-Ox nanocages exhibit superior catalytic activity stability across varied conditions, notably surpassing commercial Pt/C catalysts. Notably, achieve current densities 10 mA cm−2 at only 19.6 ± 0.1, 20.9 21.0 0.1 mV in alkaline freshwater, chemical wastewater, seawater, respectively, while maintaining satisfied with minimal loss after 40,000 cycles. situ experiments theoretical calculations reveal coordination Pt, Ru, Ni atoms creates numerous dangling bonds, which lower water dissociation barrier optimizing adsorption. This research marks a notable advancement precise engineering atomically dispersed multi-metallic centers energy-related applications. Efficient are key to economy, particularly reaction. Here, authors report offer comparable performance both freshwater wastewater conditions.

Language: Английский

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