Engineering a Copper Single‐Atom Electron Bridge to Achieve Efficient Photocatalytic CO₂ Conversion

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(13)

Опубликована: Фев. 7, 2023

Developing highly efficient and stable photocatalysts for the CO2 reduction reaction (CO2 RR) remains a great challenge. We designed Z-Scheme photocatalyst with N-Cu1 -S single-atom electron bridge (denoted as Cu-SAEB), which was used to mediate RR. The production of CO O2 over Cu-SAEB is high 236.0 120.1 μmol g-1 h-1 in absence sacrificial agents, respectively, outperforming most previously reported photocatalysts. Notably, as-designed throughout 30 cycles, totaling 300 h, owing strengthened contact interface Cu-SAEB, mediated by atomic structure. Experimental theoretical calculations indicated that SAEB greatly promoted Z-scheme interfacial charge-transport process, thus leading enhancement photocatalytic RR Cu-SAEB. This work represents promising platform development have potential conversion applications.

Язык: Английский

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Lattice Strain Engineering of Ni₂P Enables Efficient Catalytic Hydrazine Oxidation‐Assisted Hydrogen Production

Advanced Materials, Год журнала: 2023, Номер 35(42)

Опубликована: Июль 11, 2023

Hydrazine-assisted water electrolysis provides new opportunities to enable energy-saving hydrogen production while solving the issue of hydrazine pollution. Here, synthesis compressively strained Ni2 P as a bifunctional electrocatalyst for boosting both anodic oxidation reaction (HzOR) and cathodic evolution (HER) is reported. Different from multistep synthetic method that induces lattice strain by creating core-shell structures, facile strategy developed tune via dual-cation co-doping. The obtained with compressive -3.62% exhibits significantly enhanced activity HzOR HER than counterparts tensile without strain. Consequently, optimized delivers current densities 10 100 mA cm-2 at small cell voltages 0.16 0.39 V hydrazine-assisted electrolysis, respectively. Density functional theory (DFT) calculations reveal promotes dissociation concurrently tunes adsorption strength intermediates, thereby facilitating process on P. As HzOR, reduces energy barrier potential-determining step dehydrogenation *N2 H4 H3 . Clearly, this work paves pathway lattice-strained electrocatalysts

Язык: Английский

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Fullerene Lattice‐Confined Ru Nanoparticles and Single Atoms Synergistically Boost Electrocatalytic Hydrogen Evolution Reaction

Advanced Functional Materials, Год журнала: 2023, Номер 33(12)

Опубликована: Янв. 5, 2023

Abstract The design and construction of electrocatalysts with high efficiency, low cost large current output suitable for industrial hydrogen production is the development trend water electrolysis. Herein, a lattice‐confined in situ reduction effect 3D crystalline fullerene network (CFN) developed to trap Ru nanoparticle (NP) single atom (SA) via solvothermal‐pyrolysis process. optimized product (Ru NP ‐Ru SA @CFN‐800) exhibits outstanding electrocatalytic performance alkaline evolution reactions. To deliver density 10 mA cm −2 , @CFN‐800 merely required an overpotential 33 mV, along robust durability 1400 h. Even at densities 500 1000 overpotentials are only 154 251 respectively. Density function theorey calculation results indicated that electronic synergetic between enable regulate charge distribution reduce Gibbs free energy intermediate species dissociation process, thereby accelerating Moreover, CFN matrix render this strategy patulous other transition metals, e.g., Cu, Ni, Co. present study provides new clue novel electrocatalyst field storage conversion.

Язык: Английский

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Room-Temperature Laser Planting of High-Loading Single-Atom Catalysts for High-Efficiency Electrocatalytic Hydrogen Evolution

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(25), С. 13788 - 13795

Опубликована: Июнь 9, 2023

Despite stunning progress in single-atom catalysis (SAC), it remains a grand challenge to yield high loading of single atoms (SAs) anchored on substrates. Herein, we report one-step laser-planting strategy craft SAs interest under an atmospheric temperature and pressure various substrates including carbon, metals, oxides. Laser pulses render concurrent creation defects the substrate decomposition precursors into monolithic metal SAs, which are immobilized as-produced via electronic interactions. planting enables defect density, leading record-high 41.8 wt %. Our can also synthesize high-entropy (HESAs) with coexistence multiple regardless their distinct characteristics. An integrated experimental theoretical study reveals that superior catalytic activity be achieved when distribution atom content HESAs resembles performance volcano plot electrocatalysis. The noble-metal mass for hydrogen evolution reaction within is 11-fold over commercial Pt/C. robust, opening up simple general route attaining array low-cost, high-density diverse ambient conditions electrochemical energy conversion.

Язык: Английский

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Why do Single‐Atom Alloys Catalysts Outperform both Single‐Atom Catalysts and Nanocatalysts on MXene?

Angewandte Chemie International Edition, Год журнала: 2023, Номер 63(4)

Опубликована: Дек. 1, 2023

Abstract Single‐atom alloys (SAAs), combining the advantages of single‐atom and nanoparticles (NPs), play an extremely significant role in field heterogeneous catalysis. Nevertheless, understanding catalytic mechanism SAAs catalysis reactions remains a challenge compared with single atoms NPs. Herein, ruthenium‐nickel (RuNi ) synthesized by embedding atomically dispersed Ru Ni NPs are anchored on two‐dimensional Ti 3 C 2 T x MXene. The RuNi SAA‐3 −Ti catalysts exhibit unprecedented activity for hydrogen evolution from ammonia borane (AB, NH BH hydrolysis mass‐specific (r mass value 333 L min −1 g . Theoretical calculations reveal that anchoring optimizes dissociation AB H O as well binding ability H* intermediates during due to d‐band structural modulation caused alloying effect metal‐supports interactions (MSI) This work provides useful design principles developing optimizing efficient hydrogen‐related demonstrates over energy

Язык: Английский

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