General Modification Strategy on Amorphous Materials to Boost Catalytic Performance

Advanced Functional Materials, Год журнала: 2024, Номер 34(44)

Опубликована: Май 21, 2024

Abstract Amorphous materials with a high number of unsaturated coordinated dangling bonds exhibits macroscopic homogeneity and isotropy, making it easily modifiable to improve the catalytic properties. At present, several feasible modification strategies for amorphous have been proposed applied multiple fields. This review aims provide comprehensive overview recent research advancements in catalysis. First, general modifying are summarized. Subsequently, potential applications modified electrocatalysis photocatalysis highlighted. Additionally, positive effects various tools on properties elucidated. Finally, summary challenges offer critical perspective further development presented. The primary goal this is systematic understanding how enhance performance stimulate catalysts future.

Язык: Английский

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In Situ Reconstruction of Scalable Amorphous Indium-Based Metal–Organic Framework for CO₂ Electroreduction to Formate over an Ultrawide Potential Window

ACS Applied Materials & Interfaces, Год журнала: 2024, Номер 16(22), С. 28655 - 28663

Опубликована: Май 22, 2024

Amorphous metal–organic frameworks (aMOFs) are highly attractive for electrocatalytic applications due to their exceptional conductivity and abundant defect sites, but harsh preparation conditions of "top-down" strategy have hindered widespread use. Herein, the scalable production aMIL-68(In)-NH2 was successfully achieved through a facile "bottom-up" involving ligand competition with 2-methylimidazole. Multiple in situ ex characterizations reveal that evolutes into In/In2O3–x as genuine active sites during CO2 reduction (CO2RR) process. Moreover, retained amino groups could enhance adsorption. As expected, reconstructed catalyst demonstrates high formate Faradaic efficiency values (>90%) over wide potential range 800 mV flow cell, surpassing most top-ranking electrocatalysts. Density functional theory calculations oxygen vacancies induce more local charges around electroactive thereby promoting formation HCOO* intermediates. Furthermore, 16 g samples can be readily prepared one batch exhibit almost identical CO2RR performances. This work offers feasible batch-scale design amorphous MOFs efficient electrolytic CO2RR.

Язык: Английский

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Amorphous/Crystalline Interface of Bi/Bi₄NbO₈Cl Heterostructure for Improved Piezo‐Photocatalysis

Small, Год журнала: 2025, Номер unknown

Опубликована: Фев. 21, 2025

Abstract Efficient separation of photogenerated charges at the surface photocatalysts is vital for achieving high photocatalytic activity. Here, a Bi/Bi 4 NbO 8 Cl heterostructure piezo‐photocatalyst with an amorphous/crystalline interface (acBi/BNC) prepared by in situ reduction using Bi as self‐sacrificial template. This ingenious design synergistically utilizes advantages structure, localized plasmon resonance effect, and piezoelectric field. The formation interfaces induces generation oxygen vacancies, subsequently lattice distortions, thus improving properties. Theoretical experimental results demonstrate that combination field promotes effective migration between bulk catalysts. Under simultaneous light ultrasound, optimal (acBi/BNC‐3) exhibit superior photodegradation efficiency tetracycline reached 80% within 5 min, reaction rate (2.78 × 10 −1 min ) 7.8 5.4 times pure (BNC) crystalline (cBi/BNC), respectively. Furthermore, piezo‐photocatalytic degradation surpasses those under individual photocatalysis piezocatalysis conditions. work provides novel rational to improve spatial charge Bi‐based catalysts prepare high‐performance piezo‐photocatalysts via engineering.

Язык: Английский

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Anion-Mediated In Situ Reconstruction of the Bi₂MoO₆ Precatalyst for Enhanced Electrochemical CO₂ Reduction over a Wide Potential Window

ACS Applied Materials & Interfaces, Год журнала: 2023, Номер 16(1), С. 742 - 751

Опубликована: Дек. 18, 2023

Electrochemical CO2 reduction reaction (eCO2RR) is a viable approach to achieve carbon neutrality. Bismuth-based electrocatalysts demonstrate exceptional selectivity in CO2-to-formate conversion, but their reconstruction mechanisms during the eCO2RR remain elusive. Herein, processes of bismuth molybdate (Bi2MoO6) nanoplates are elucidated eCO2RR. Operando and ex situ measurements reveal partial Bi2MoO6 Bi metal, forming Bi@Bi2MoO6 at negative potentials. Meanwhile, CO32– ions electrolyte spontaneously exchange with MoO42– Bi2MoO6. The obtained Bi@Bi2MoO6/Bi2O2CO3 delivers formate Faradaic efficiency (FE) 95.2% −1.0 V. Notably, high FEs (>90%) maintained within wide 500 mV window. Although computational calculations indicate higher energy barrier for *OCHO formation on Bi2O2CO3, prevention excessive metal significantly enhances long-term stability. Furthermore, ion process occurs various 2D Bi-containing precatalysts, which should be emphasized further studies.

Язык: Английский

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Constructing Cu⁰/Cu⁺ interfaces on Cu-based MOF derivatives to promote the adsorption stability of intermediates in the process of CO₂ electroreduction to C₂ products

Environmental Science Nano, Год журнала: 2024, Номер 11(10), С. 4230 - 4239

Опубликована: Янв. 1, 2024

The unique Cu 0 /Cu + interface of Cu-MOF74/Cu 2 O-350 enhances the adsorption reaction intermediates and provides more active sites, thereby increasing faradaic efficiency (FE) CO reduction to C H 4 .

Язык: Английский

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Reduced Graphene Oxide Regulates Indium Oxide In-Situ Reconstruction for Enhanced CO₂ Electroreduction

ACS Materials Letters, Год журнала: 2025, Номер unknown, С. 796 - 803

Опубликована: Янв. 31, 2025

The practical application of electrocatalytic CO2 reduction requires adaptation to the fluctuating voltage output photovoltaic systems. However, potential-induced in-situ reconstruction catalyst complicates control and leads Faradaic efficiency (FE) instability across potential window. Here, we present a redox graphene-supported indium oxide (G-InOx), where rGO effectively regulates surface evolution InOx from In3+ In0 during reactions. multivalent In generated via lowers energy barriers for *OCHO formation dissociation, enhancing formate production. also environment, optimizing proton delivery active sites. Over wide range (−0.86 −1.37 V vs RHE), G-InOx achieves FEformate nearly 100%. This work offers straightforward efficient strategy scalable, high-performance electroreduction.

Язык: Английский

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Regulating p-orbital of metallic bismuth nanosheets via transition-metal oxides enables advanced CO2 electroreduction

Science China Materials, Год журнала: 2024, Номер 67(6), С. 1965 - 1974

Опубликована: Май 11, 2024

Язык: Английский

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Modulating the Active Sites of VS₂ by Mn Doping for Highly Selective CO₂ Electroreduction to Methanol in a Flow Cell

ACS Applied Materials & Interfaces, Год журнала: 2024, Номер 16(28), С. 36453 - 36461

Опубликована: Июль 1, 2024

Methanol is a valuable liquid C1 product in CO2 electroreduction (CO2ER); however, it hard to achieve high selectivity and large current density simultaneously. In this work, we construct Mn2+-doped VS2 multilayer nanowafers applied flow cell yield methanol as single tackle challenge. Mn doping adjusts the electronic structure of concurrently introduces sulfur vacancies, forming critical *COB intermediate facilitating its sequential hydrogenation methanol. The optimal Mn4.8%-VS2 exhibits Faradic efficiencies more than 60% over wide potential range -0.4 -0.8 V cell, which maximal value 72.5 ± 1.1% at -0.6 along with partial 74.3 1.1 mA cm-2. This work opens an avenue rationally design catalysts for engineering intermediates toward CO2ER cell.

Язык: Английский

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Progress in Catalysts for Formic Acid Production by Electrochemical Reduction of Carbon Dioxide

Topics in Current Chemistry, Год журнала: 2024, Номер 383(1)

Опубликована: Дек. 3, 2024

Язык: Английский

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Rational Design of Amorphous Nanomaterials for Enhanced Electrochemical CO₂ and Nitrate Reduction

ChemCatChem, Год журнала: 2024, Номер unknown

Опубликована: Апрель 26, 2024

Abstract Amorphous materials are distinguished by their exceptional attributes, notably expansive surface area and the profusion of active sites they present. Consequently, amorphization process stands as an efficacious strategy to augment catalytic efficacy electrocatalysts. This is achieved through meticulous construction architecture precise modulation electronic configuration these materials. Therefore, this review aims offer a thorough examination latest progress in application amorphous for enhancement electrocatalytic processes, with particular emphasis on nitrate (NO 3 − ) reduction reaction (NITRR) carbon dioxide (CO 2 RR). Initially, we delve into structural benefits inherent materials, outlining diverse synthesis techniques characterization methodologies utilized development. Following this, illustrate utilization various NITRR CO RR, accentuating how framework influences activities. Concludingly, encapsulate merits obstacles encountered electrocatalysts whilst also forecasting future direction creation innovative

Язык: Английский

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