| 1. |
- Wu, Yunzhen, et al.
(författare)
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Beyond d Orbits : Steering the Selectivity of Electrochemical CO(2)Reduction via Hybridized sp Band of Sulfur-Incorporated Porous Cd Architectures with Dual Collaborative Sites
- 2020
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Ingår i: Advanced Energy Materials. - : Wiley. - 1614-6832 .- 1614-6840. ; 10:45
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Tidskriftsartikel (refereegranskat)abstract
- Electrochemical CO(2)reduction is regarded as a promising strategy for the sustainable conversion of greenhouse gas. However, it still remains a significant challenge to manipulate the selectivity and activity. Herein, amorphous and porous Cd modified by sulfur (P-Cd|S) is synthesized by a p-block sulfur dopant. In comparison with unmodified Cd metal, the P-Cd|S architecture exhibits superior activity for selective CO generation, indicating that the sulfur dopant enables a selectivity shift from formic acid to CO. The high selectivity of P-Cd|S is partially ascribed to the local alkalization and suppression of hydrogen evolution as indicated by the finite element analysis. In-depth mechanistic investigations by operando Raman, Infrared, and X-ray photoelectron spectroscopy in combination with theory calculations indicate that the covalently hybridized sp band system with dual collaborative sites (Cd(delta)(+)and S-delta(-)) gives rise to a strong interplay with CO(2)molecules and carbonaceous species, leading to the natural elimination of linear correlation among intermediates binding for d-band metals and the convenient modulation of selectivity toward CO versus HCOOH.
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| 2. |
- Zhai, Panlong, et al.
(författare)
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Engineering active sites on hierarchical transition bimetal oxides/sulfides heterostructure array enabling robust overall water splitting
- 2020
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Ingår i: Nature Communications. - : Springer Nature. - 2041-1723. ; 11:1
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Tidskriftsartikel (refereegranskat)abstract
- Rational design of the catalysts is impressive for sustainable energy conversion. However, there is a grand challenge to engineer active sites at the interface. Herein, hierarchical transition bimetal oxides/sulfides heterostructure arrays interacting two-dimensional MoOx/MoS2 nanosheets attached to one-dimensional NiOx/Ni3S2 nanorods were fabricated by oxidation/hydrogenation-induced surface reconfiguration strategy. The NiMoOx/NiMoS heterostructure array exhibits the overpotentials of 38mV for hydrogen evolution and 186mV for oxygen evolution at 10mAcm(-2), even surviving at a large current density of 500mAcm(-2) with long-term stability. Due to optimized adsorption energies and accelerated water splitting kinetics by theory calculations, the assembled two-electrode cell delivers the industrially relevant current densities of 500 and 1000mAcm(-2) at record low cell voltages of 1.60 and 1.66V with excellent durability. This research provides a promising avenue to enhance the electrocatalytic performance of the catalysts by engineering interfacial active sites toward large-scale water splitting. While water splitting is an appealing carbon-neutral strategy for renewable energy generation, there is a need to develop new active, cost-effective catalysts. Here, authors prepare a nickel-molybdenum oxide/sulfide heterojunctions as bifunctional H-2 and O-2 evolution electrocatalysts.
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