Desalination, Год журнала: 2025, Номер unknown, С. 118630 - 118630
Опубликована: Янв. 1, 2025
Язык: Английский
ACS Nano, Год журнала: 2023, Номер 17(21), С. 20804 - 20824
Опубликована: Ноя. 3, 2023
The splitting of water through electrocatalysis offers a sustainable method for the production hydrogen. In alkaline electrolytes, lack protons forces dissociation to occur before hydrogen evolution reaction (HER). While pure Pt is gold standard electrocatalyst in acidic since 5d orbital nearly fully occupied, when it overlaps with molecular water, generates Pauli repulsion. As result, formation Pt–H* bond an environment difficult, which slows HER and negates benefits using catalyst. To overcome this limitation, can be alloyed transition metals, such as Fe, Co, Ni. This approach has potential not only enhance performance but also increase dispersion decrease its usage, thus overall improving catalyst's cost-effectiveness. excellent adsorption ability metals contributes generation proton-rich local near Pt-based alloy that promotes HER. Significant progress been achieved comprehending mechanism manipulation structure composition electrocatalysts based on alloy. objective review analyze condense latest developments It focuses modified alloys clarifies design principles catalytic catalysts from both experimental theoretical perspective. highlights some difficulties encountered during opportunities increasing performance. Finally, guidance development more efficient provided.
Язык: Английский
Процитировано
92
Coordination Chemistry Reviews, Год журнала: 2023, Номер 499, С. 215492 - 215492
Опубликована: Окт. 27, 2023
Язык: Английский
Процитировано
66
Advanced Science, Год журнала: 2024, Номер 11(19)
Опубликована: Март 14, 2024
Abstract Developing cost‐efficient trifunctional catalysts capable of facilitating hydrogen evolution reaction (HER), oxygen (OER), and reduction (ORR) activity is essential for the progression energy devices. Engineering these to optimize their active sites integrate them into a cohesive system presents significant challenge. This study introduces nanoflower (NFs)‐like carbon‐encapsulated FeNiPt nanoalloy catalyst (FeNiPt@C NFs), synthesized by substituting Co 2+ ions with high‐spin Fe in Hofmann‐type metal‐organic framework, followed carbonization pickling processes. The FeNiPt@C NFs catalyst, characterized its nitrogen‐doped metal alloy structure phase‐segregated slight surface oxidization, exhibits excellent catalytic performance. evidenced activities HER (−25 mV at 10 mA cm −2 ), ORR (half‐wave potential 0.93 V), OER (294 enhanced water oxidation attributed state element. Consequently, Zn‐air battery anion exchange membrane electrolyzer assembled demonstrate remarkable power density (168 mW ) industrial‐scale current (698 1.85 respectively. innovative integration multifunctional paves way advancement sustainable systems.
Язык: Английский
Процитировано
59
Advanced Energy Materials, Год журнала: 2023, Номер 13(46)
Опубликована: Окт. 27, 2023
Abstract Precisely designing asymmetric diatomic configurations and studying their electronic regulation effect for improving the oxygen reduction reaction (ORR) performance are important anion exchange membrane fuel cells (AEMFCs). Here, a Fe, Cu co‐doped 2D crystalline IISERP‐MOF27 nanosheet derived FeN 3 O‐CuN 4 site nanocatalyst (named as FeCu‐NC) is synthesized cathodes of AEMFCs. Thanks to optimal structure in FeCu‐NC catalyst, it shows enhanced half‐wave potential (0.910 V), turnover frequency (0.165e s −1 ), decreased activation energy (19.96 kJ mol ) KOH. The FeCu‐NC‐based AEMFC achieves extremely high kinetic current (0.138 A cm −2 at 0.9 V) rated power density (1.09 W surpassing best‐reported transition metal‐based cathodes. Density functional theory calculations further demonstrate that Cu‐N can break localization Fe‐3d orbitals, accelerate electron transport, optimize OH adsorption, thus facilitating ORR process.
Язык: Английский
Процитировано
54
ACS Nano, Год журнала: 2024, Номер 18(5), С. 4308 - 4319
Опубликована: Янв. 23, 2024
The intrinsic roadblocks for designing promising Pt-based oxygen reduction reaction (ORR) catalysts emanate from the strong scaling relationship and activity–stability–cost trade-offs. Here, a carbon-supported Pt nanoparticle Mn single atom (PtNP–MnSA/C) as in situ constructed PtNP–MnSA pairs are demonstrated to be an efficient catalyst circumvent above seesaws with only ∼4 wt % loadings. Experimental theoretical investigations suggest that MnSA functions not "assist" sites cooperatively facilitate dissociation of O2 due electronic polarization, affording dissociative pathway reduced H2O2 production, but also structure "modulator" downshift d-band center sites, alleviating overbinding oxygen-containing intermediates. More importantly, serves "stabilizer" endow PtNP–MnSA/C excellent structural stability low Fenton-like reactivity, resisting fast demetalation metal sites. As result, PtNPs–MnSA/C shows ORR performance half-wave potential 0.93 V vs reversible hydrogen electrode high mass activity 1.77 A/mgPt at 0.9 acid media, which is 19 times higher than commercial Pt/C declines by 5% after 80,000 cycles. Specifically, reaches power density 1214 mW/cm2 2.87 A/cm2 H2–O2 fuel cell.
Язык: Английский
Процитировано
43
Journal of the American Chemical Society, Год журнала: 2024, Номер 146(3), С. 2132 - 2140
Опубликована: Янв. 16, 2024
The direct pyrolysis of metal-zeolite imidazolate frameworks (M-ZIFs) has been widely recognized as the predominant approach for synthesizing atomically dispersed metal–nitrogen-carbon single-atom catalysts (M/NC-SACs), which have exhibited exceptional activity and selectivity in semihydrogenation acetylene. However, due to weak adsorption reactants on single site restricted molecular diffusion, large organic molecules (e.g., phenylacetylene) was greatly limited M/NC-SACs. In this work, a dual catalyst (h–Pd-Mn/NC) with hollow mesopores designed prepared using general host–guest strategy. Taking phenylacetylene an example, ultrahigh selectivity, achieved turnover frequency 218 molC═CmolPd–1 min–1, 16-fold higher than that commercial Lindlar catalyst. maintained high even after 5 cycles usage. superior h–Pd-Mn/NC attributed 4.0 nm mesopore interface catalyst, enhanced diffusion macromolecular products. Particularly, introduction Mn electronegativity could drive electron transfer from adjacent Pd sites regulate electronic structure sites. Meanwhile, strong coupling Pd–Mn pairs d-electron domination near Fermi level promoted H2 active sites, thereby reducing energy barrier phenylacetylene.
Язык: Английский
Процитировано
42
Advanced Powder Materials, Год журнала: 2024, Номер 3(2), С. 100170 - 100170
Опубликована: Янв. 3, 2024
Modulating electronic structures of single-atom metal cocatalysts is vital for highly active photoreduction CO2, and it's especially challenging to develop a facile method modify the dispersion atomical photocatalytic sites. We herein report an ion-loading pyrolysis route in-situ anchor Pd single atoms as well twinned nanoparticles on ultra-thin graphitic carbon nitride nanosheets (PdTP/PdSA-CN) high-efficiency CO2. The anchored donate electrons adjacent Pd–N4 sites through networks, optimized PdTP/PdSA-CN photocatalyst exhibits CO evolution rate up 46.5 μmol g−1 h−1 with nearly 100 % selectivity. As revealed by spectroscopic theoretical analyses, superior activity attributed lowered desorption barrier carbonyl species at electron-enriched atoms, together improved efficiencies light-harvesting charge separation/transport. This work has demonstrated engineering electron density assisted strong interaction support atomic metal, unveiled underlying mechanism expedited efficiency.
Язык: Английский
Процитировано
27
Advanced Functional Materials, Год журнала: 2024, Номер 34(36)
Опубликована: Март 18, 2024
Abstract Recently, a diverse array of novel metal‐nitrogen‐carbon (M‐N‐C) single‐atom catalysts (SACs) have rapidly evolve, particularly in the realm oxygen reduction reaction (ORR). Despite plethora proposed design and improvement strategies for SACs, comprehensive review systematically compiling components M‐N‐C from unified perspective is notably absent. For first time, thorough examination each component conducted, focusing on entropy increase active sites SACs. single M‐N 4 whole system, an implies elevated degree disorder chaos. Broadly, entropy‐increasing modification M (single mental sites) guest groups entails augmentation chaos, with most effective co‐catalytic synergy achieved by establishing multiple through “cocktail effect”. Concerning N (nitrogen other heteroatoms) C (carbon supports), induces heightened disorder, symmetry breaking more likely to drive toward adsorbing molecules attain equilibrium symmetric structure. All these innovative led remarkable ORR activity stability offer guiding criterion future preparation
Язык: Английский
Процитировано
27
Chinese Chemical Letters, Год журнала: 2024, Номер unknown, С. 109557 - 109557
Опубликована: Янв. 1, 2024
Язык: Английский
Процитировано
26
Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер 347, С. 123792 - 123792
Опубликована: Апрель 24, 2024
Язык: Английский
Процитировано
26