Isolated Metal Centers Activate Small Molecule Electrooxidation: Mechanisms and Applications DOI Open Access
Yanmin Hu,

Tingting Chao,

Yuhai Dou

и другие.

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 26, 2025

Abstract Electrochemical oxidation of small molecules shows great promise to substitute oxygen evolution reaction (OER) or hydrogen (HOR) enhance kinetics and reduce energy consumption, as well produce high‐valued chemicals serve fuels. For these reactions, high‐valence metal sites generated at oxidative potentials are typically considered active trigger the process molecules. Isolated atom site catalysts (IASCs) have been developed an ideal system precisely regulate state coordination environment single‐metal centers, thus optimize their catalytic property. The isolated in IASCs inherently possess a positive state, can be more readily homogeneous under than nanoparticle counterparts. Meanwhile, merely centers but lack ensemble sites, which alter adsorption configurations compared with counterparts, induce various pathways mechanisms change product selectivity. More importantly, construction is discovered limit d‐electron back donation CO 2p * orbital overly strong on resolve poisoning problems most electro‐oxidation reactions improve stability. Based advantages fields electrochemical molecules, this review summarizes recent developments advancements focusing anodic HOR fuel cells OER electrolytic alternative such formic acid/methanol/ethanol/glycerol/urea/5‐hydroxymethylfurfural (HMF) key reactions. merits different decoding structure–activity relationships specifically discussed guide precise design structural regulation from perspective comprehensive mechanism. Finally, future prospects challenges put forward, aiming motivate application possibilities for diverse functional IASCs.

Язык: Английский

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

и другие.

Advanced Energy Materials, Год журнала: 2024, Номер 14(30)

Опубликована: Май 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.

Язык: Английский

Процитировано

43
Seawater electrolysis for fuels and chemicals production: fundamentals, achievements, and perspectives DOI
Lin Chen,

Chang Yu,

Junting Dong

и другие.

Chemical Society Reviews, Год журнала: 2024, Номер 53(14), С. 7455 - 7488

Опубликована: Янв. 1, 2024

Seawater electrolysis for the production of fuels and chemicals involved in onshore offshore plants powered by renewable energies offers a promising avenue unique advantages energy environmental sustainability. Nevertheless, seawater presents long-term challenges issues, such as complex composition, potential side reactions, deposition poisoning microorganisms metal ions, well corrosion, thus hindering rapid development technology. This review focuses on value-added (hydrogen beyond) fine through electrolysis, step towards sustainable carbon neutrality. The principle related are first introduced, redox reaction mechanisms summarized. Strategies operating anodes cathodes including application chloride- impurity-resistant electrocatalysts/membranes reviewed. We comprehensively summarize (hydrogen, monoxide, sulfur, ammonia,

Язык: Английский

Процитировано

38
Bimetallic NiCo Metal–Organic Frameworks with High Stability and Performance Toward Electrocatalytic Oxidation of Urea in Seawater DOI

Soheila Sanati,

Reza Abazari, Alexander M. Kirillov

и другие.

Inorganic Chemistry, Год журнала: 2024, Номер 63(34), С. 15813 - 15820

Опубликована: Авг. 14, 2024

The urea oxidation reaction (UOR) is an alternative anodic for hydrogen generation via water splitting. significance of UOR lies in both H2 production and the decontamination urea-containing wastewater. Commercial electrocatalysts this field are generally based on noble metals show several limitations. Bimetal–organic frameworks (BMOFs) can be excellent candidates replacement noble-metal-based catalysts beacuse their promising features, such as a tunable structure, high surface area, abundant sites electrocatalysis. In study, series nickel–cobalt BMOFs (Nix-Coy-BMOFs: x y refer to molar fraction Ni Co) were synthesized applied UOR. particular, Ni0.15Co0.85-MOF material with structure similar that its parent Co-MOF, revealed exceptional electrocatalytic performance, evidenced by low values overpotential (1.33 V vs RHE at 10 mA cm–2), TOF (0.47 s–1), Tafel slope (125 mV dec–1). At 40 cm–2 current density, also showed stability during 72 h tests. This performance NiCo-BMOF assigned synergistic effect between Co Ni, active sites, porosity, all which result increased rate due acceleration charge mass transfers. Thus, present work introduces efficient noble-metal-free energy from urea-based

Язык: Английский

Процитировано

24
Sustainable Carbon‐Based Catalyst Materials Derived From Lignocellulosic Biomass for Energy Storage and Conversion: Atomic Modulation and Properties Improvement DOI Creative Commons
Wei Li, Ying Xu, Guanhua Wang

и другие.

Carbon Energy, Год журнала: 2025, Номер unknown

Опубликована: Март 20, 2025

ABSTRACT Carbon electrocatalyst materials based on lignocellulosic biomass with multi‐components, various dimensions, high carbon content, and hierarchical morphology structures have gained great popularity in electrocatalytic applications recently. Due to the catalytic deficiency of neutral atoms, usage single lignocellulosic‐based electrocatalysis involving energy storage conversion presents unsatisfactory applicability. However, atomic‐level modulation lignocellulose‐based can optimize electronic structures, charge separation, transfer processes, so forth, which results substantially enhanced performance carbon‐based catalysts. This paper reviews recent advances rational design as electrocatalysts from an perspective, such self/external heteroatom doping metal modification. Then, through systematic discussion principles reaction mechanisms catalysts, prepared catalysts rechargeable batteries are reviewed. Finally, challenges improving prospects diverse review contributes synthesis strategy via modulation, turn promotes lignocellulose valorization for conversion.

Язык: Английский

Процитировано

3
Artificial Heterointerfaces with Regulated Charge Distribution of Ni Active Sites for Urea Oxidation Reaction DOI
Lei Chen, Lei Wang, Jin‐Tao Ren

и другие.

Small Methods, Год журнала: 2024, Номер unknown

Опубликована: Апрель 1, 2024

Abstract In contrast to the thermodynamically unfavorable anodic oxygen evolution reaction, electrocatalytic urea oxidation reaction (UOR) presents a more favorable thermodynamic potential. However, practical application of UOR has been hindered by sluggish kinetics. this study, hierarchical porous nanosheet arrays featuring abundant Ni‐WO 3 heterointerfaces on nickel foam (Ni‐WO /NF) is introduced as monolith electrode, demonstrating exceptional activity and stability toward UOR. The /NF catalyst exhibits unprecedentedly rapid kinetics (200 mA cm −2 at 1.384 V vs. RHE) high turnover frequency (0.456 s −1 ), surpassing most previously reported Ni‐based catalysts, with negligible decay observed during durability test lasting 150 h. Ex situ X‐ray photoelectron spectroscopy density functional theory calculations elucidate that WO interface significantly modulates local charge distribution Ni species, facilitating generation 3+ optimal affinity for interacting molecules CO 2 intermediates This mechanism accelerates interfacial Additionally, in Fourier transform infrared provides deep insights into substantial contribution sites electrocatalysis, unraveling underlying molecular‐level mechanisms. Finally, study explores direct fuel cell inspire future implementations.

Язык: Английский

Процитировано

17
Engineering active sites on binary metal selenide heterointerface catalyst to boost urea electrooxidation DOI
Felix Ofori Boakye, Marshet Getaye Sendeku, Anuj Kumar

и другие.

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер 352, С. 124013 - 124013

Опубликована: Апрель 21, 2024

Язык: Английский

Процитировано

17
Nickel Hydroxide‐Based Electrocatalysts for Promising Electrochemical Oxidation Reactions: Beyond Water Oxidation DOI
Hainan Sun, Sanzhao Song

Small, Год журнала: 2024, Номер 20(33)

Опубликована: Март 20, 2024

Transition metal hydroxides have attracted significant research interest for their energy storage and conversion technique applications. In particular, nickel hydroxide (Ni(OH)

Язык: Английский

Процитировано

15
Fe-Doped Ni2P/NiSe2 Composite Catalysts for Urea Oxidation Reaction (UOR) for Energy-Saving Hydrogen Production by UOR-Assisted Water Splitting DOI

Chen‐Jin Huang,

Qi‐Ni Zhan,

Huimin Xu

и другие.

Inorganic Chemistry, Год журнала: 2024, Номер 63(19), С. 8925 - 8937

Опубликована: Апрель 29, 2024

The development of efficient urea oxidation reaction (UOR) catalysts helps UOR replace the oxygen evolution (OER) in hydrogen production from water electrolysis. Here, we prepared Fe-doped Ni2P/NiSe2 composite catalyst (Fe–Ni2P/NiSe2-12) by using phosphating-selenizating and acid etching to increase intrinsic activity active areas. Spectral characterization theoretical calculations demonstrated that electrons flowed through Ni–P–Fe–interface–Ni–Se–Fe, thus conferring high Fe–Ni2P/NiSe2-12, which only needed 1.39 V vs RHE produce current density 100 mA cm–2. Remarkably, this potential was 164 mV lower than required for OER under same conditions. Furthermore, EIS driven Fe–Ni2P/NiSe2-12 exhibited faster interfacial reactions, charge transfer, response compared OER. Consequently, can effectively prevent competition with NSOR, making it suitable UOR-assisted Notably, when electrolysis is operated at a 40 cm–2, system achieve decrease 140 traditional This study presents novel strategy splitting energy-saving production.

Язык: Английский

Процитировано

15
Regulating Reconstruction‐Engineered Active Sites for Accelerated Electrocatalytic Conversion of Urea DOI Creative Commons
Jichao Zhang, Jianrui Feng, Jiexin Zhu

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(36)

Опубликована: Июнь 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

Язык: Английский

Процитировано

14
Microenvironment Engineering of Heterogeneous Catalysts for Liquid-Phase Environmental Catalysis DOI

Zhong‐Shuai Zhu,

Shuang Zhong, Cheng Cheng

и другие.

Chemical Reviews, Год журнала: 2024, Номер 124(20), С. 11348 - 11434

Опубликована: Окт. 9, 2024

Environmental catalysis has emerged as a scientific frontier in mitigating water pollution and advancing circular chemistry reaction microenvironment significantly influences the catalytic performance efficiency. This review delves into engineering within liquid-phase environmental catalysis, categorizing microenvironments four scales: atom/molecule-level modulation, nano/microscale-confined structures, interface surface regulation, external field effects. Each category is analyzed for its unique characteristics merits, emphasizing potential to enhance efficiency selectivity. Following this overview, we introduced recent advancements advanced material system design promote (e.g., purification, transformation value-added products, green synthesis), leveraging state-of-the-art technologies. These discussions showcase was applied different reactions fine-tune regimes improve from both thermodynamics kinetics perspectives. Lastly, discussed challenges future directions engineering. underscores of intelligent materials drive development more effective sustainable solutions decontamination.

Язык: Английский

Процитировано

14