RhNi Bimetallenes with Lattice‐Compressed Rh Skin towards Ultrastable Acidic Nitrate Electroreduction

Advanced Materials, Год журнала: 2024, Номер 36(23)

Опубликована: Фев. 26, 2024

Harvesting recyclable ammonia (NH

Язык: Английский

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Electronic Structure Design of Transition Metal-Based Catalysts for Electrochemical Carbon Dioxide Reduction

ACS Nano, Год журнала: 2024, Номер 18(14), С. 9823 - 9851

Опубликована: Март 28, 2024

With the increasingly serious greenhouse effect, electrochemical carbon dioxide reduction reaction (CO2RR) has garnered widespread attention as it is capable of leveraging renewable energy to convert CO2 into value-added chemicals and fuels. However, performance CO2RR can hardly meet expectations because diverse intermediates complicated processes, necessitating exploitation highly efficient catalysts. In recent years, with advanced characterization technologies theoretical simulations, exploration catalytic mechanisms gradually deepened electronic structure catalysts their interactions intermediates, which serve a bridge facilitate deeper comprehension structure-performance relationships. Transition metal-based (TMCs), extensively applied in CO2RR, demonstrate substantial potential for further modulation, given abundance d electrons. Herein, we discuss representative feasible strategies modulate catalysts, including doping, vacancy, alloying, heterostructure, strain, phase engineering. These approaches profoundly alter inherent properties TMCs interaction thereby greatly affecting rate pathway CO2RR. It believed that rational design modulation fundamentally provide viable directions development toward conversion many other small molecules.

Язык: Английский

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Electrocatalytic Nitrate Reduction on Metallic CoNi‐Terminated Catalyst with Industrial‐Level Current Density in Neutral Medium

Advanced Materials, Год журнала: 2024, Номер 36(30)

Опубликована: Май 9, 2024

Abstract Green ammonia synthesis through electrocatalytic nitrate reduction reaction (eNO 3 RR) can serve as an effective alternative to the traditional energy‐intensive Haber‐Bosch process. However, achieving high Faradaic efficiency (FE) at industrially relevant current density in neutral medium poses significant challenges eNO RR. Herein, with guidance of theoretical calculation, a metallic CoNi‐terminated catalyst is successfully designed and constructed on copper foam, which achieves FE up 100% under industrial‐level very low overpotential (−0.15 V versus reversible hydrogen electrode) medium. Multiple characterization results have confirmed that maintained metal atom‐terminated surface interaction atoms plays crucial role reducing density. By constructing homemade gas stripping absorption device, complete conversion process for high‐purity ammonium products demonstrated, displaying potential practical application. This work suggests sustainable promising toward directly converting nitrate‐containing pollutant solutions into nitrogen fertilizers.

Язык: Английский

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Modulating the Electrolyte Microenvironment in Electrical Double Layer for Boosting Electrocatalytic Nitrate Reduction to Ammonia

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(32)

Опубликована: Май 29, 2024

Abstract Electrochemical nitrate reduction reaction (NO 3 RR) is a promising approach to achieve remediation of nitrate‐polluted wastewater and sustainable production ammonia. However, it still restricted by the low activity, selectivity Faraday efficiency for ammonia synthesis. Herein, we propose an effective strategy modulate electrolyte microenvironment in electrical double layer (EDL) mediating alkali metal cations enhance NO RR performance. Taking bulk Cu as model catalyst, experimental study reveals that − ‐to‐NH performance different electrolytes follows trend Li + <Cs <Na <K . Theoretical studies illustrate proton transport rate activity rate‐determining step 2 ) increase order The cation effects are also general two typical nanostructured catalysts including copper/cuprous oxide nickel phosphides, achieving near‐100 % Faradaic over 99 conversion NH Furthermore, demonstrate can be converted high‐purity 4 Cl catalyst K ‐containing electrolyte.

Язык: Английский

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Enhancing Compatibility of Two‐Step Tandem Catalytic Nitrate Reduction to Ammonia Over P‐Cu/Co(OH)₂

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Сен. 11, 2024

Abstract Electrochemical nitrate reduction reaction (NO 3 RR) is a promising approach to realize ammonia generation and wastewater treatment. However, the transformation from NO − NH involves multiple proton‐coupled electron transfer processes by‐products 2 , H etc.), making high selectivity challenge. Herein, two‐phase nanoflower P‐Cu/Co(OH) electrocatalyst consisting of P‐Cu clusters P‐Co(OH) nanosheets designed match two‐step tandem process ) more compatible, avoiding excessive accumulation optimizing whole reaction. Focusing on initial 2e process, inhibited * desorption Cu sites in gives rise appropriate released electrolyte. Subsequently, exhibits superior capacity for trapping transforming desorbed during latter 6e due thermodynamic advantage contributions active hydrogen. In 1 m KOH + 0.1 leads yield rate 42.63 mg h cm Faradaic efficiency 97.04% at −0.4 V versus reversible hydrogen electrode. Such well‐matched achieves remarkable synthesis performance perspective catalytic reaction, offering novel guideline design RR electrocatalysts.

Язык: Английский

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In-situ exsolution of FeCo nanoparticles over perovskite oxides for efficient electrocatalytic nitrate reduction to ammonia via localized electrons

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер 357, С. 124267 - 124267

Опубликована: Июнь 5, 2024

Язык: Английский

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Co‐Catalytic Metal‐Support Interactions Design on Single‐Atom Alloy for Boosted Electro‐Reduction of Nitrate to Nitrogen

Advanced Functional Materials, Год журнала: 2024, Номер 34(45)

Опубликована: Май 28, 2024

Abstract The past decades have seen considerable imbalances in the nitrogen cycle due to excessive use of nitrate agriculture and industry. Electrocatalytic reduction (NO 3 RR) (N 2 ) holds significant potential for addressing pollution wastewater but suffers from nitrite formation sluggish hydrogeneration process. Here a single atom alloy (SAA) catalyst featuring atomically dispersed Ru on 2D Ni metal (Ru 1 Ni), proving remarkable performance − –N conversion (≈93%) N selectivity (≈99%)) through co‐catalytic metal‐support interactions (CMSI) effect is reported. Significantly, SAA achieves NO RR removal capacity as high 11.1 mg L −1 h cm −2 with 20 cycles stability (9 per cycle), surpassing most previously reported works. core boosting lies synergistically promoted activation accelerated hydrogenation oxide intermediates site substrate, respectively, revealed by various situ experiments theoretical simulations. DFT calculations indicate electron transfer substrate more robust interaction between Ru–Ni comparison that Ni–Ni. This work offers resilient methodology rational design highly efficient electrocatalysts CMSI modulation RR, illuminating arena treatment cycle.

Язык: Английский

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Regulating the Electrochemical Nitrate Reduction Performance with Controllable Distribution of Unconventional Phase Copper on Alloy Nanostructures

Advanced Materials, Год журнала: 2024, Номер unknown

Опубликована: Сен. 6, 2024

Abstract Electrochemical nitrate reduction reaction (NO 3 RR) is emerging as a promising strategy for removal and ammonia (NH ) production using renewable electricity. Although great progresses have been achieved, the crystal phase effect of electrocatalysts on NO RR remains rarely explored. Here, epitaxial growth unconventional 2H Cu hexagonal close‐packed ( hcp IrNi template, resulting in formation three IrNiCu@Cu nanostructures, reported. IrNiCu@Cu‐20 shows superior catalytic performance, with NH Faradaic efficiency (FE) 86% at −0.1 (vs reversible hydrogen electrode [RHE]) yield rate 687.3 mmol g −1 h , far better than common face‐centered cubic Cu. In sharp contrast, IrNiCu@Cu‐30 IrNiCu@Cu‐50 covered by shell display high selectivity toward nitrite 2 − ), FE above 60% 0.1 RHE). Theoretical calculations demonstrated that has optimal electronic structures due to highest d‐band center strongest trend lowest energy barriers. The electroactivity originates from abundant low coordination sites surface, which guarantees fast electron transfer accelerate intermediate conversions. This work provides feasible tactic regulate product distribution engineering electrocatalysts.

Язык: Английский

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Precise synthesis of dual atom sites for electrocatalysis

Nano Research, Год журнала: 2024, Номер unknown

Опубликована: Сен. 17, 2024

Язык: Английский

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Interfacial Water Regulation for Nitrate Electroreduction to Ammonia at Ultralow Overpotentials

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 8, 2025

Abstract Nitrate electroreduction is promising for achieving effluent waste‐water treatment and ammonia production with respect to the global nitrogen balance. However, due impeded hydrogenation process, high overpotentials need be surmounted during nitrate electroreduction, causing intensive energy consumption. Herein, a hydroxide regulation strategy developed optimize interfacial H 2 O behavior accelerating conversion of at ultralow overpotentials. The well‐designed Ru─Ni(OH) electrocatalyst shows remarkable efficiency 44.6% +0.1 V versus RHE nearly 100% Faradaic NH 3 synthesis 0 RHE. In situ characterizations theoretical calculations indicate that Ni(OH) can regulate structure promoted dissociation process contribute spontaneous hydrogen spillover boosting NO − Ru sites. Furthermore, assembled rechargeable Zn‐NO /ethanol battery system exhibits an outstanding long‐term cycling stability charge–discharge tests high‐value‐added ammonium acetate, showing great potential simultaneously removal, conversion, chemical synthesis. This work not only provide guidance in extensive reactions but also inspire design novel hybrid flow multiple functions.

Язык: Английский

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