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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Promoting Electroreduction of CO₂ and NO₃⁻ to Urea via Tandem Catalysis of Zn Single Atoms and In₂O_3‐x

Advanced Energy Materials, Год журнала: 2024, Номер unknown

Опубликована: Авг. 16, 2024

Abstract Urea electrosynthesis from co‐electrolysis of CO 2 and NO 3 − (UECN) offers an innovative route for converting waste /NO into valuable urea. Herein, Zn single atoms anchored on oxygen vacancy (OV)‐rich In O 3‐x (Zn 1 /In ) are developed as a highly active selective UECN catalyst, delivering the highest urea yield rate 41.6 mmol h −1 g urea‐Faradaic efficiency 55.8% at −0.7 V in flow cell, superior to most previously reported catalysts. situ spectroscopic measurements theoretical calculations unveil synergy In/Zn sites OVs promoting process via tandem catalysis mechanism, where ‐OV site activates form * NH while In‐OV CO. The formed spontaneously migrates nearby then couples with generate CONH which is ultimately converted

Язык: Английский

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Synergistic Cu Single Atoms and MoS₂‐Edges for Tandem Electrocatalytic Reduction of NO₃⁻ and CO₂ to Urea

Advanced Energy Materials, Год журнала: 2024, Номер 14(43)

Опубликована: Авг. 16, 2024

Abstract Urea electrosynthesis from co‐electrolysis of NO 3 − and CO 2 (UENC) under ambient conditions is recognized as an appealing approach for effective sustainable urea production, while it requires high‐efficiency UENC electrocatalysts to promote the C─N coupling hydrogenation processes. Herein, single‐atom Cu anchored on MoS (Cu 1 ‐MoS ) explored a highly active selective catalyst. Theoretical calculations operando spectroscopic characterizations unveil synergistic tandem catalysis UENC, where single atoms trigger early coupling, ‐edges key step * NH COOHNH generation. Strikingly, equipped in flow cell achieves excellent performance with maximum urea‐Faradaic efficiency 57.02% at −0.6 V corresponding yield rate 23.3 mmol h −1 g , surpassing nearly all previously reported catalysts.

Язык: Английский

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Spin State Modulation with Oxygen Vacancy Orientates C/N Intermediates for Urea Electrosynthesis of Ultrahigh Efficiency

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 23, 2025

Abstract The co‐electrolysis of CO 2 and NO 3 − to synthesize urea has become an effective pathway alternate the conventional Bosch‐Meiser process, while complexity C‐/N‐containing intermediates for C−N coupling results in electrosynthesis unsatisfactory efficiency. In this work, electronic spin state modulation maneuver with oxygen vacancies (Ov) is unveiled effectively meliorate oriented generation key * NH coupling, furnishing ultrahigh yield 2175.47 µg mg −1 h Faraday efficiency 70.1%. Mechanistic studies expound that Ov can induce conversion high‐spin Ni 2+ (t 2g 6 e g ) Ni@CeO 2−x low‐spin 3+ 1 ), which markedly enhances hybridization degree 3d N 2p orbitals NO, facilitating selective formation . Notably, situ generated serve as a localized proton donor promote electroreduction on adjacent site Ce −O exclusively afford CO, followed by each other efficiently urea. strategy tailored switching active provides reliable reference rectify structure electrocatalysts directional valorization.

Язык: Английский

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Selective Urea Electrosynthesis from Nitrate and CO₂ on Isolated Copper Alloyed Ruthenium

ACS Energy Letters, Год журнала: 2024, Номер 9(9), С. 4624 - 4632

Опубликована: Авг. 30, 2024

Urea electrosynthesis by coelectrolysis of NO3– and CO2 (UENC) represents a promising method to enable efficient sustainable urea production. In this work, isolated Cu alloyed Ru (Cu1Ru) is developed as highly active selective UENC catalyst. Combined theoretical computations in situ spectroscopic measurements reveal the synergistic effect Cu1–Ru site Ru–Ru on Cu1Ru promote via tandem catalysis pathway, which drives *NO2/CO2 coupling followed *CO2NO2-to-*CO2NH step. The formed *CO2NH then migrates from adjacent promotes *CO2NH⃗*CO2NH2 → *COOHNH2 steps toward generation. Impressively, achieves high performance flow cell, exhibiting yield rate 21.04 mmol h–1 gcat–1 Faradaic efficiency 51.27% at −0.6 V, outperforming most reported catalysts.

Язык: Английский

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Electrocatalytic Urea Production with Nitrate and CO₂ on a Ru‐Dispersed Co Catalyst

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Авг. 12, 2024

Abstract Urea electrosynthesis from co‐electrolysis of NO 3 − and CO 2 (UENC) provides an alternative route for realizing efficient sustainable urea production. In this work, single‐atom Ru dispersed on Co (Ru 1 Co) is demonstrated as effective robust catalyst the UENC. situ spectroscopic measurements theoretical simulations unravel cooperative effect sites to promote UENC process via a tandem catalysis mechanism, where site activates adsorption hydrogenation form * NH , while hydrogenation/deoxygenation CO. The generated then transferred nearby which promotes C─N coupling toward formation. Strikingly, assembled in flow cell shows highest urea‐Faradaic efficiency 50.1% with corresponding yield rate 22.34 mmol h −1 g at −0.5 V (RHE), superior most reported catalysts

Язык: Английский

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Boosted Nitrate and CO₂ Reduction for Urea Electrosynthesis on p-Block Bi Dispersed Ru Alloys

ACS Sustainable Chemistry & Engineering, Год журнала: 2025, Номер unknown

Опубликована: Фев. 10, 2025

Язык: Английский

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Advances in rare earth catalysts for small molecule electrosynthesis☆

Journal of Rare Earths, Год журнала: 2025, Номер unknown

Опубликована: Фев. 1, 2025

Язык: Английский

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Asymmetric CuS₁N₄ as Axial Polarization Site Trigger Rapid Charge Transport Channels for Boosting Photosynthesis of Ammonia

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 10, 2025

Abstract Effective photogenerated charge transfer and utilization have been regarded as a critical factor for achieving highly efficient photosynthesis of ammonia. However, the lacks necessary driving force in many catalysts limit directly transfer. In this work, Cu porphyrin‐based monoatomic layer (PML‐Cu) is modified on face‐centered cubic structured defective CdIn 2 S 4 via solvothermal reaction, with strong coupled interfacial Cu─S bond constructed. Owing to formation axial CuS 1 N polarization site, local asymmetric configuration can be created between PML‐Cu form potential difference, inducing rapid transport from bond. Meantime, electron‐enriched site beneficial stabilization * NHOH intermediate state, then lowering NHO→ rate‐limiting step energy barrier. Benefiting these features, PML‐Cu/CdIn exhibit good NH 3 generation rate 1979.0 µmol g −1 h , apparent quantum efficiency 8.56% at 380 nm 7.40% 450 nm, respectively. This work provides an accessible pathway designing coupling boost photocatalysis.

Язык: Английский

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A multi-site Ru-Cu/CeO2 photocatalyst for boosting C-N coupling toward urea synthesis

Science Bulletin, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

Язык: Английский

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