Photocatalysis of water into hydrogen peroxide over an atomic Ga-N5 site

Nature Synthesis, Год журнала: 2023, Номер 2(6), С. 557 - 563

Опубликована: Март 27, 2023

Язык: Английский

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Phosphorus Tailors thed‐Band Center of Copper Atomic Sites for Efficient CO₂Photoreduction under Visible‐Light Irradiation

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(38)

Опубликована: Июль 8, 2022

Photoreduction of CO2 into solar fuels has received great interest, but suffers from low catalytic efficiency and poor selectivity. Herein, two single-Cu-atom catalysts with unique Cu configurations in phosphorus-doped carbon nitride (PCN), namely, Cu1 N3 @PCN P3 were fabricated via selective phosphidation, tested visible light-driven reduction by H2 O without sacrificial agents. was exclusively active for CO production a rate 49.8 μmolCO gcat-1 h-1 , outperforming most polymeric (C3 N4 ) based catalysts, while preferably yielded . Experimental theoretical analysis suggested that doping P C3 replacing corner C atom upshifted the d-band center close to Fermi level, which boosted adsorption activation on making efficiently convert CO. In contrast, much lower 3d electron energy exhibited negligible adsorption, thereby preferring formation photocatalytic splitting.

Язык: Английский

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Integrating Single Atoms with Different Microenvironments into One Porous Organic Polymer for Efficient Photocatalytic CO₂ Reduction

Advanced Materials, Год журнала: 2021, Номер 33(33)

Опубликована: Июль 8, 2021

Abstract The precise identification of single‐atom catalysts (SACs) activity and boosting their efficiency toward CO 2 conversion is imperative yet quite challenging. Herein, for the first time a series porous organic polymers designed prepared simultaneously, containing well‐defined M–N 4 O sites. Such strategy not only offers multiactive sites to promote catalytic but also provides more direct chance identify metal center activity. photoreduction results indicate that introduction salphen unit with Ni–N centers into pristine phthalocyanine‐based framework achieves remarkable generation ability (7.77 mmol g –1 ) high selectivity 96% over H . In combination control experiments, as well theoretical studies, moiety evidenced active site RR compared traditional moiety, which can be ascribed effectively reducing energy barrier, facilitating adsorption reaction radicals *COOH, improving charge transportation. This work might shed some light on designing efficient SACs reduction through modification coordination environments.

Язык: Английский

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Review of Carbon Support Coordination Environments for Single Metal Atom Electrocatalysts (SACS)

Advanced Materials, Год журнала: 2023, Номер 36(1)

Опубликована: Апрель 20, 2023

This topical review focuses on the distinct role of carbon support coordination environment single-atom catalysts (SACs) for electrocatalysis. The article begins with an overview atomic configurations in SACs, including a discussion advanced characterization techniques and simulation used understanding active sites. A summary key electrocatalysis applications is then provided. These processes are oxygen reduction reaction (ORR), evolution (OER), hydrogen (HER), nitrogen (NRR), dioxide (CO

Язык: Английский

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Loading Single‐Ni Atoms on Assembled Hollow N‐Rich Carbon Plates for Efficient CO₂ Electroreduction

Advanced Materials, Год журнала: 2021, Номер 34(1)

Опубликована: Окт. 7, 2021

The rational design of catalysts' spatial structure is vitally important to boost catalytic performance through exposing the active sites, enhancing mass transfer, and confining reactants. Herein, a dual-linker zeolitic tetrazolate framework-engaged strategy developed construct assembled hollow plates (AHP) N-rich carbon (NC), which loaded with single-Ni atoms form highly efficient electrocatalyst (designated as Ni-NC(AHP)). In carbonization process, thermally unstable linker (5-aminotetrazole) serves self-sacrificial template other (2-methylimidazole) mainly nitrogen source NC matrix. formed Ni-NC(AHP) catalyst possesses enhanced mesoporosity more available surface area, thus promoting transport affording abundant accessible sites. These features contribute remarkable for electrochemical CO2 reduction exceptionally high selectivity nearly 100% towards CO in wide potential range dramatically partial current density.

Язык: Английский

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Fabrication and regulation of vacancy-mediated bismuth oxyhalide towards photocatalytic application: Development status and tendency

Coordination Chemistry Reviews, Год журнала: 2021, Номер 443, С. 214033 - 214033

Опубликована: Май 25, 2021

Язык: Английский

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Carbon Nanocage with Maximum Utilization of Atomically Dispersed Iron as Efficient Oxygen Electroreduction Nanoreactor

Advanced Materials, Год журнала: 2022, Номер 35(5)

Опубликована: Ноя. 9, 2022

As key parameters of electrocatalysts, the density and utilization active sites determine electrocatalytic performance toward oxygen reduction reaction. Unfortunately, prevalent electrocatalysts fail to maximize due inappropriate nanostructural design. Herein, a nano-emulsion induced polymerization self-assembly strategy is employed prepare hierarchical meso-/microporous N/S co-doped carbon nanocage with atomically dispersed FeN4 (denoted as Meso/Micro-FeNSC). In situ scanning electrochemical microscopy technology reveals available for Meso/Micro-FeNSC reach 3.57 × 1014 cm-2 , representing more than threefold improvement compared micropore-dominant Micro-FeNSC counterpart (1.07 ). Additionally, turnover frequency also improved 0.69 from 0.50 e- site-1 s-1 Micro-FeNSC. These properties motivate efficient electroreduction electrocatalyst, in terms outstanding half-wave potential (0.91 V), remarkable kinetic mass specific activity (68.65 A g-1 ), excellent robustness. The assembled Zn-air batteries deliver high peak power (264.34 mW large capacity (814.09 mA h long cycle life (>200 h). This work sheds lights on quantifying site significance maximum rational design advanced catalysts.

Язык: Английский

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Mesoporous N‐rich Carbon with Single‐Ni Atoms as a Multifunctional Sulfur Host for Li‐S Batteries

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(47)

Опубликована: Сен. 27, 2022

Physicochemical confinement and catalytic conversion of lithium polysulfides (LiPSs) are crucial to suppress the shuttle effect enhance redox kinetics lithium-sulfur (Li-S) batteries. In this study, a NH4 Cl-assisted pyrolysis strategy is developed fabricate highly mesoporous N-rich carbon (designed as NC(p)) featuring thin outer shells porous inner networks, on which single-Ni atoms anchored form an excellent sulfur host Ni-NC(p)) for Li-S During pyrolysis, pyrolytic HCl from confined Cl within ZIF-8 will in situ etch produce rich carbonized product NC(p). The Ni-NC(p) enables favorable electron/ion transfer, high loading, effective LiPSs, while species enhances LiPSs. As result, cathode based delivers obviously improved battery performance with specific capacity, good rate capability, cycling stability.

Язык: Английский

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Optimizing the semiconductor–metal-single-atom interaction for photocatalytic reactivity

Nature Reviews Chemistry, Год журнала: 2022, Номер 6(11), С. 823 - 838

Опубликована: Окт. 24, 2022

Язык: Английский

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Synthesis of N‐Doped Highly Graphitic Carbon Urchin‐Like Hollow Structures Loaded with Single‐Ni Atoms towards Efficient CO₂Electroreduction

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(18)

Опубликована: Фев. 23, 2022

The rational design of single-atom catalysts featuring excellent conductivity, highly accessible discrete active sites and favorable mass transfer is crucial for electrocatalysis but remains challenging. In this study, a reliable Ni-catalyzed Ni-templated strategy developed to synthesize catalyst by transforming metallic Ni into single-Ni atoms anchored on hollow porous urchin-like (HPU) N-doped carbon (NC) (designated as Ni-NC(HPU)), which possesses high crystallinity sufficient Ni-N4 moiety (2.4 wt %). unique thorns the surface, good conductivity large external surface area facilitate electron/mass exposure sites. As result, Ni-NC(HPU) exhibits remarkable activity stability CO2 electroreduction. Moreover, synthetic can also be facilely extended prepare distinct architectures with similar components, such wire- sphere-like ones.

Язык: Английский

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