Energy & Environmental Science, Год журнала: 2024, Номер 17(16), С. 6024 - 6033
Опубликована: Янв. 1, 2024
A H-buffer chain by exploiting the oxygen diversity of confined polyoxometalates to accelerate H-spillover on Pt in HER is designed. typical pathway (Pt → O br O3H Mo/W c PC sub-1-nm ) revealed, which can buffer H-migration barriers.
Язык: Английский
Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(42)
Опубликована: Сен. 2, 2023
Abstract Designing novel single‐atom catalysts (SACs) supports to modulate the electronic structure is crucial optimize catalytic activity, but rather challenging. Herein, a general strategy proposed utilize metalloid properties of trap and stabilize single‐atoms with low‐valence states. A series supported on surface tungsten carbide (M‐WC x , M=Ru, Ir, Pd) are rationally developed through facile pyrolysis method. Benefiting from WC exhibit weak coordination W C atoms, resulting in formation active centers similar metals. The unique metal‐metal interaction effectively stabilizes single atoms improves orbital energy level distribution sites. As expected, representative Ru‐WC exhibits superior mass activities 7.84 62.52 mg Ru −1 for hydrogen oxidation evolution reactions (HOR/HER), respectively. In‐depth mechanistic analysis demonstrates that an ideal dual‐sites cooperative mechanism achieves suitable adsorption balance H ad OH energetically favorable Volmer step. This work offers new guidance precise construction highly SACs.
Язык: Английский
Процитировано
114
Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(12)
Опубликована: Янв. 30, 2024
Abstract Efficient dual‐single‐atom catalysts are crucial for enhancing atomic efficiency and promoting the commercialization of fuel cells, but addressing sluggish kinetics hydrogen oxidation reaction (HOR) in alkaline media facile site generation remains formidable challenges. Here, we break local symmetry ultra‐small ruthenium (Ru) nanoparticles by embedding cobalt (Co) single atoms, which results release Ru atoms from on reduced graphene oxide (Co 1 1,n /rGO). In situ operando spectroscopy theoretical calculations reveal that oxygen‐affine Co atom disrupts nanoparticles, resulting parasitic within nanoparticles. The interaction between forms effective active centers. parasitism modulates adsorption OH intermediates sites, accelerating HOR through faster formation *H 2 O. As anticipated, /rGO exhibits ultrahigh mass activity (7.68 A mg −1 ) at 50 mV exchange current density (0.68 mA cm −2 ), 6 7 times higher than those Ru/rGO, respectively. Notably, it also displays exceptional durability surpassing commercial Pt catalysts. This investigation provides valuable insights into hybrid multi‐single‐atom metal nanoparticle catalysis.
Язык: Английский
Процитировано
76
Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(16)
Опубликована: Фев. 29, 2024
Abstract Alkaline water electrolysis (AWE) plays a crucial role in the realization of hydrogen economy. The design and development efficient stable bifunctional catalysts for both evolution reaction (HER) oxygen (OER) are pivotal to achieving high‐efficiency AWE. Herein, WC 1‐x /Mo 2 C nanoparticle‐embedded carbon nanofiber (WC C@CNF) with abundant interfaces is successfully designed synthesized. Benefiting from electron transfer behavior Mo , electrocatalysts C@CNF exhibit superior HER OER performance. Furthermore, when employed as anode cathode membrane electrode assembly devices, catalyst exhibits enhanced catalytic activity remarkable stability 100 hours at high current density 200 mA cm −2 towards overall splitting. experimental characterizations theoretical simulation reveal that modulation d‐band center C@CNF, achieved through asymmetric charge distribution resulting built‐in electric field induced by work function, enables optimization adsorption strength hydrogen/oxygen intermediates, thereby promoting kinetics This provides promising strategies designing highly active energy conversion fields.
Язык: Английский
Процитировано
76
Advanced Energy Materials, Год журнала: 2024, Номер 14(28)
Опубликована: Март 3, 2024
Abstract Electrochemically reducing nitrate (NO 3 − ), a common water pollutant, to valuable ammonia (NH ) offers green, sustainable, and decentralized route for synthesis. Electrochemical reduction reaction RR) involves two crucial steps: deoxygenation followed by nitrite hydrogenation; in particular, the hydrogenation is rate‐determining step (RDS) NO RR. In this work, an atomically dispersed cobalt‐phosphorus (Co─P) catalytic pair (CP) with strong electronic coupling reported. The Co site Co─P CP effectively activates , while P facilitates dissociation release H + synergistically enhancing thermodynamic kinetic performance of electrochemical ammonia.
Язык: Английский
Процитировано
76
Advanced Functional Materials, Год журнала: 2023, Номер 33(36)
Опубликована: Май 14, 2023
Abstract Rhenium disulfide (ReS 2 ) holds expansive perspective in photocatalytic water‐splitting field, but its H ‐production rate is severely impeded by the strong hydroxyl (OH ad adsorption on catalytic Re atoms. Herein, an ingenious strategy about charging d ‐orbital electrons of ReS 2+x cocatalyst integrating metallic Au explicitly clarified to effectively accelerate OH desorption for promoting alkaline ‐evolution activity. To this end, core‐shell Au@ReS nanostructures as cocatalysts are skillfully fabricated onto TiO a directional assembly pathway. Experimental and theoretical data validate free‐electron transfer from core S‐rich shell, thus essentially d‐orbital atoms construct active (4‐ δ )+ sites. The charged electron state raises antibonding occupancy OH bonds, thereby accelerating endowing efficient production water splitting. Moreover, can capture photogenerated unveiled operando Kelvin probe force microscopy. Consequently, optimized /Au@ReS photocatalyst achieves exceptional 6013.45 µmol h −1 g with releasing visual bubbles media. This research furnishes original insights orbital optimize strength between intermediates
Язык: Английский
Процитировано
64
Advanced Materials, Год журнала: 2023, Номер 36(13)
Опубликована: Дек. 16, 2023
Anionic modification engineering is a crucial approach to develop highly efficient electrocatalysts for hydrogen evolution reaction. Herein, halogen elements (X = Cl, Br, and I)-modified Ru-based nanosheets (X-Ru/RuP
Язык: Английский
Процитировано
59
Advanced Functional Materials, Год журнала: 2024, Номер 34(24)
Опубликована: Янв. 7, 2024
Abstract Resourceful and inexpensive seawater direct splitting omits the desalination process effectively increases efficiency of hydrogen energy generation. However, development is hampered by competing selectivity challenges from anodic oxygen evolution reaction (OER) chlorine issues electrode corrosion. Herein, borate anion‐intercalated NiV‐LDH nanoflakes/NiCoP nanowires heterostructures supported on Ni foam (2D/1D NiV‐BLDH/NiCoP/NF) synthesized. Theoretical calculations show that a small amount V atom doping in Ni(OH) 2 favorable for changing electronic environment around atoms via bridging Ni─O, which can construct Ni─O─V to accelerate electron transfer promote catalytic activity. The anions (B(OH) 4 − ) intercalation not only results good hydrophilicity high OH but also weakens adsorption (Cl ), restrains reaction. Thus, component optimized NiV 0.1 ‐BLDH/NiCoP/NF electrocatalyst requires 268 mV overpotential reach 100 mA cm −2 OER an alkaline environment. Particularly, NiCoP/NF||NiV cell exhibits attractive overall water performance with low voltage 1.46 1.53 at 10 freshwater seawater, respectively. design strategy this provides new avenue splitting.
Язык: Английский
Процитировано
51
Chemical Society Reviews, Год журнала: 2024, Номер 53(12), С. 6021 - 6041
Опубликована: Янв. 1, 2024
This review provides a comprehensive overview of the recent advancements in controllable synthesis high-entropy alloys, ranging from approach and significance composition, morphology, structure, surface/interface engineering.
Язык: Английский
Процитировано
27
Small, Год журнала: 2024, Номер 20(27)
Опубликована: Янв. 28, 2024
Low-cost bifunctional electrocatalysts capable of efficiently driving the hydrogen evolution reaction (HER) and oxygen (OER) are needed for growth a green economy. Herein, Ru/Co
Язык: Английский
Процитировано
20
Advanced Functional Materials, Год журнала: 2024, Номер 34(48)
Опубликована: Июль 5, 2024
Abstract Cobalt single atom catalysts (SACs) have exhibited promising performance in both the oxygen reduction reaction (ORR) and evolution (OER), positioning them as potential dual‐functional for Zn‐air battery. However, long‐standing challenge lies achieving satisfactory dual‐functionality stability of these SACs. In this study, to optimize 4e ‒ ORR performance, boron (B) atoms are employed with low electronegativity regulate structure Co–N–C catalytic center. This resulted formation an asymmetrically coordinated Co metal center catalyst (Co‐N 3 B). Compared Co‐N 4 , B lower free energy stronger adsorption toward * O species, effectively suppressing 2e pathway at cobalt site preventing corrosion induced by hydrogen peroxide (H 2 ) reactions, thereby enhancing stability. situ attenuated total reflectance surface‐enhanced infrared absorption spectroscopy (ATR‐SEIRAS) further validated excellent interaction between active centers intermediates. Furthermore, self‐made rechargeable zinc‐air battery demonstrated remarkable discharge peak power density (≈253 mW cm ‒2 ), (≈819 mAh g ‒1 cyclic exceeding 110 h. study provides new insights into constructing atomic‐level precision offers strong references practical applications storage convension electrocatalysts.
Язык: Английский
Процитировано
19