Dual Functions of CO2 Molecular Activation and 4f Levels as Electron Transport Bridge in Dysprosium Single Atom Composite Photocatalysts with Enhanced Visible‐Light Photoactivities
Abstract:Environmental and energy issues are the two main challenges that hinder the sustainable development of human society. [1][2][3][4][5][6] Solar energy has attracted urgent attention due to
“…44,[71][72][73] CO 2 reduction,45,62,[74][75][76] N 2 reduction,63,77,78 C-O coupling,65 pollutant degradation, 79,80 CH 4 conversion,68 H 2 O 2 production,69 as well as photocatalytic sensing 70,81,82. …”
“…44,[71][72][73] CO 2 reduction,45,62,[74][75][76] N 2 reduction,63,77,78 C-O coupling,65 pollutant degradation, 79,80 CH 4 conversion,68 H 2 O 2 production,69 as well as photocatalytic sensing 70,81,82. …”
“…The large atomic radius of Gd results in quite a small number of Gd atoms being loaded into CB. [18] On the contrary, the graphite stripes disappear and the new Ni (111) crystal planes emerge in CBNNiGd-700 and CBNNi-700, implying that Ni with the relatively small atomic radius is readily incorporated into the graphite lattices of CB, which can generate defect sites. [23] As revealed by the elemental mapping images, Ni atoms agglomerate into nanoparticles encapsulated in the carbon matrixes of CBNNiGd-700 and CBNNi-700, [11] while the relatively uniform dispersion of Gd atoms is accomplished within CBNNiGd-700 and CBNGd-700.…”
Section: Resultsmentioning
confidence: 99%
“…[17] Recent reports have demonstrated that LMs can be loaded onto various supports and employed in a variety of catalytic reactions. [18,19] LMs with the comparatively large ion radii are able to induce lattice distortion and deformation stress of supports, conducive to the formation of defect sites. [19] In the meantime, the strong lanthanide contraction effect of LM atoms can change the local electron densities of the surrounding atoms and optimize the electronic states of the supports, in favor of the elevation of adsorption capabilities of catalyst surfaces and thereby the strengthening of catalytic performance.…”
Generally, in terms of electrocatalytic CO 2 reduction, single-atom catalysts show high selectivities yet low current densities whereas conventional nanoparticle catalysts exhibit relatively high current densities but low selectivities. This work combines the advantages of the two classes of catalysts by constructing a Ni-Gd-N-doped carbon black electrocatalyst within which Ni I active sites are exposed outside the carbon layers and Ni nanoparticles are encapsulated inside the carbon layers. The Gd atoms can not only influence the local electron densities of Ni 3d orbitals, thus strengthening the electronic activity, but also tailor the sizes of the Ni nanoparticles, thereby minimizing the activity toward hydrogen evolution. Accordingly, this electrocatalyst yields both a high CO faradaic efficiency (97 %) and a large current density (308 mA cm À 2 ), alongside an outstanding stability (100 h).
“…As another excellent catalyst material, CdS has been widely used in hydrogen production from water splitting and photocatalytic degradation of organic pollutants. [29][30][31][32][33] CdS has high visible light response and carrier transport ability. More importantly, the suitable band gap (2.4 eV) of CdS can be well matched with that of InVO 4 ; so it is possible to form a Type-II heterostructure.…”
By taking advantage of the unique advantages of Eu3+ single atom catalysis and the II-type heterojunction in the field of photocatalytic reduction, a Eu3+ single atom doped CdS/InVO4 II-type heterojunction was successfully constructed.
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