Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 307, С. 121190 - 121190
Опубликована: Фев. 8, 2022
Язык: Английский
Chemical Reviews, Год журнала: 2024, Номер 124(7), С. 3694 - 3812
Опубликована: Март 22, 2024
Electrocatalytic water splitting driven by renewable electricity has been recognized as a promising approach for green hydrogen production. Different from conventional strategies in developing electrocatalysts the two half-reactions of (e.g., and oxygen evolution reactions, HER OER) separately, there growing interest designing bifunctional electrocatalysts, which are able to catalyze both OER. In addition, considering high overpotentials required OER while limited value produced oxygen, is another rapidly exploring alternative oxidation reactions replace hybrid toward energy-efficient generation. This Review begins with an introduction on fundamental aspects splitting, followed thorough discussion various physicochemical characterization techniques that frequently employed probing active sites, emphasis reconstruction during redox electrolysis. The design, synthesis, performance diverse based noble metals, nonprecious metal-free nanocarbons, overall acidic alkaline electrolytes, thoroughly summarized compared. Next, their application also presented, wherein anodic include sacrificing agents oxidation, pollutants oxidative degradation, organics upgrading. Finally, concise statement current challenges future opportunities presented hope guiding endeavors quest sustainable
Язык: Английский
Процитировано
268
Advanced Functional Materials, Год журнала: 2023, Номер 33(12)
Опубликована: Янв. 15, 2023
Abstract Electrochemical reduction of nitrate to ammonia (NO 3 RR) holds a great promise for attaining both NH electrosynthesis and wastewater purification. Herein, single‐atom Bi alloyed Pd metallene (Bi 1 Pd) is reported as highly effective NO RR catalyst, showing near 100% ‐Faradaic efficiency with the corresponding yield 33.8 mg h −1 cm −2 at −0.6 V versus RHE, surpassing those almost all ever catalysts. In‐depth theoretical operando spectroscopic investigations unveil that electronically couples its neighboring atoms synergistically activate − destabilize *NO on Pd, leading reduced energy barrier potential‐determining step (*NO→*NOH) enhanced protonation energetics ‐to‐NH pathway.
Язык: Английский
Процитировано
238
Nature Communications, Год журнала: 2022, Номер 13(1)
Опубликована: Март 3, 2022
Abstract Developing high-performance electrocatalysts for hydrogen evolution reaction (HER) is crucial sustainable production, yet still challenging. Here, we report boron-modulated osmium (B-Os) aerogels with rich defects and ultra-fine diameter as a pH-universal HER electrocatalyst. The catalyst shows the small overpotentials of 12, 19, 33 mV at current density 10 mA cm −2 in acidic, alkaline, neutral electrolytes, respectively, well excellent stability, surpassing commercial Pt/C. Operando X-ray absorption spectroscopy that interventional interstitial B atoms can optimize electron structure B-Os stabilize Os active sites an electron-deficient state under realistic working conditions, simultaneously reveals catalytic mechanisms electrolytes. functional theory calculations also indicate introducing tailor electronic Os, resulting reduced water dissociation energy improved adsorption/desorption behavior hydrogen, which synergistically accelerate HER.
Язык: Английский
Процитировано
233
ACS Catalysis, Год журнала: 2021, Номер 11(23), С. 14338 - 14351
Опубликована: Ноя. 12, 2021
The development of high-performance electrocatalysts is a highly efficient strategy to optimize the sluggish kinetic property oxygen evolution reaction (OER). Herein, we synthesize kind nickel foam (NF)-supported electrocatalyst composed one-dimensional Co3O4 nanowire as core and two-dimensional NiFe-LDH nanosheet shell (denoted NiFe-60/Co3O4@NF). Fluorine introduced into precursor Co(OH)F Co3O4, which results in improved thermal stability significantly increased regularly distributed vacancies, while electrochemically deposited nanosheets possess crystalline/amorphous hybrid structure. As result, hetero-interface mainly constituting Ni species from contributes interaction between Co Fe facilitates electron transfer. Simultaneously, vacancies coordinatively unsaturated amorphous area also determined, finally completing backtracking. Benefiting these factors, only low overpotentials 221 257 mV are required deliver current densities 100 500 mA cm–2, respectively, with quite small Tafel slope 34.6 dec–1 during OER for well-designed NiFe-60/Co3O4@NF electrocatalyst.
Язык: Английский
Процитировано
211
Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 306, С. 121097 - 121097
Опубликована: Янв. 13, 2022
Язык: Английский
Процитировано
185
Advanced Materials, Год журнала: 2023, Номер 35(12)
Опубликована: Янв. 4, 2023
Developing highly efficient multifunctional electrocatalysts is crucial for future sustainable energy pursuits, but remains a great challenge. Herein, facile synthetic strategy used to confine atomically thin Pd-PdO nanodomains amorphous Ru metallene oxide (RuO2 ). The as-synthesized electrocatalyst (Pd2 RuOx-0.5 h) exhibits excellent catalytic activity toward the pH-universal hydrogen evolution reaction (η10 = 14 mV in 1 m KOH, η10 12 0.5 H2 SO4 , and 22 PBS), alkaline oxygen 225 mV), overall water splitting (E10 1.49 V) with high mass operational stability. Further reduction endows material RuOx-2 promising activity, evidenced by halfway potential, four-electron selectivity, poison tolerance. enhanced attributed rational integration of favorable nanostructures, including 1) nanosheet morphology, 2) coexisting defective crystalline phases, 3) multi-component heterostructural features. These structural factors effectively regulate material's electronic configuration adsorption intermediates at active sites energetics.
Язык: Английский
Процитировано
174
Advanced Materials, Год журнала: 2021, Номер 34(5)
Опубликована: Окт. 22, 2021
Next-generation batteries based on conversion reactions, including aqueous metal-air batteries, nonaqueous alkali metal-O2 and -CO2 metal-chalcogen metal-ion have attracted great interest. However, their use is restricted by inefficient reversible of active agents. Developing bifunctional catalysts to accelerate the reaction kinetics in both discharge charge processes urgently needed. Graphene-, or graphene-like carbon-supported atomically dispersed metal (G-ADMCs) been demonstrated show excellent activity various electrocatalytic making them promising candidates. Different from G-ADMCs for catalysis, which only require high one direction, rechargeable should provide discharging charging. This review provides guidance design fabrication next-generation reactions. The key challenges that prevent conversion, origin G-ADMCs, current principles highly analyzed highlighted each conversion-type battery. Finally, a summary outlook development G-ADMC materials with energy density efficiency are given.
Язык: Английский
Процитировано
171
ACS Nano, Год журнала: 2022, Номер 16(11), С. 17847 - 17890
Опубликована: Окт. 31, 2022
Over the past few decades, development of electrocatalysts for energy applications has extensively transitioned from trial-and-error methodologies to more rational and directed designs at atomic levels via either nanogeometric optimization or modulating electronic properties active sites. Regarding modulation properties, nonprecious transition metal-based materials have been attracting large interest due capability versatile tuning d-electron configurations expressed through flexible orbital occupancy various possible degrees spin polarization. Herein, recent advances in tailoring transition-metal atoms intrinsically enhanced electrocatalytic performances are reviewed. We start with discussions on how polarization can govern essential level processes, including transport electron charge bulk, reactive species adsorption catalytic surface, transfer between centers adsorbed as well reaction mechanisms. Subsequently, different techniques currently adopted structures discussed particular emphasis theoretical rationale practical achievements. also highlight promises recently established computational design approaches developing applications. Lastly, discussion is concluded perspectives current challenges future opportunities. hope this review will present beauty structure–activity relationships catalysis sciences contribute advance conversion
Язык: Английский
Процитировано
144
Carbon Energy, Год журнала: 2023, Номер 5(12)
Опубликована: Апрель 4, 2023
Abstract Small‐molecule electrooxidation‐boosted water electrolysis (WE) is an energy‐saving method for hydrogen (H 2 ) production. Herein, PdPt bimetallenes (PdPt BMLs) are obtained through the simple galvanic replacement reaction. BMLs reveal 2.93‐fold enhancement in intrinsic electroactivity and 4.53‐fold mass formate oxidation reaction (FOR) with respect to Pd metallenes (Pd MLs) at 0.50 V potential due synergistic effect. Meanwhile, introduction of Pt atoms also considerably increases evolution (HER) MLs alkaline medium, which even exceeds that use commercial nanocrystals. Inspired by outstanding FOR HER bifunctional BMLs, a two‐electrode FOR‐boosted WE system (FOR‐WE) constructed using as cathode anode. The FOR‐WE only requires operational voltage 0.31 achieve H production, 1.48 lower than (ca. 1.79 V) traditional system.
Язык: Английский
Процитировано
143
Advanced Functional Materials, Год журнала: 2023, Номер 33(45)
Опубликована: Сен. 1, 2023
Abstract Oxygen evolution reaction (OER) remains a bottleneck for electrocatalytic water‐splitting to generate hydrogen. However, the traditional adsorbed mechanism (AEM) possesses sluggish kinetics due scaling relationship, while lattice oxygen (LOM) triggers an unstable structure escaping of oxygen. Herein, proof‐of‐concept Fe‐Co(OH) 2 /Fe O 3 heterostructure is put forward, where following AEM can complete rapidly deprotonation process Fe LOM trigger O─O coupling step. Combining theoretical and experimental investigation confirmed that redistributed space‐charge junction optimize synergistically oxygen, facilitate synchronously OER activity stability. As result, shows excellent performance with low overpotential only 219 249 mV reach current density 10 100 mA cm −2 . Specifically, electrocatalyst maintains long‐term stability h at large This work paves avenue break through limit conventional mechanism.
Язык: Английский
Процитировано
127