2020
DOI: 10.1002/anie.202004510
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Regulating Charge Transfer of Lattice Oxygen in Single‐Atom‐Doped Titania for Hydrogen Evolution

Abstract: Single‐atom catalysts have attracted much attention. Reported herein is that regulating charge transfer of lattice oxygen atoms in serial single‐atom‐doped titania enables tunable hydrogen evolution reaction (HER) activity. First‐principles calculations disclose that the activity of lattice oxygen for the HER can be regularly promoted by substituting its nearest metal atom, and doping‐induced charge transfer plays an essential role. Besides, the realm of the charge transfer of the active site can be enlarged t… Show more

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Cited by 60 publications
(41 citation statements)
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“…[ 13 ] The central metal layer in MPS 3 is enclosed by S and P, [ 14 ] partial substitution of the central metal by a different transition metal element would enrich its electronic structure, which has been demonstrated with increased electrocatalytic performance. [ 15–19 ] For example, iron has been utilized to partially substitute the nickel atom in NiPS 3 with the formation of Fe‐doped NiPS 3 nanosheets (NSs) exhibiting an increased electrochemical activity towards OER with reduced overpotential from 0.353 to 0.256 V. The introduction of Fe reduces the combination of oxygen‐containing species and NiPS 3 , thereby lowering the reaction energy barrier during OER. [ 17 ] Such electronic engineering by modifying the surface adsorption energy may also be accomplished by the anionic exchange.…”
Section: Introductionmentioning
confidence: 99%
“…[ 13 ] The central metal layer in MPS 3 is enclosed by S and P, [ 14 ] partial substitution of the central metal by a different transition metal element would enrich its electronic structure, which has been demonstrated with increased electrocatalytic performance. [ 15–19 ] For example, iron has been utilized to partially substitute the nickel atom in NiPS 3 with the formation of Fe‐doped NiPS 3 nanosheets (NSs) exhibiting an increased electrochemical activity towards OER with reduced overpotential from 0.353 to 0.256 V. The introduction of Fe reduces the combination of oxygen‐containing species and NiPS 3 , thereby lowering the reaction energy barrier during OER. [ 17 ] Such electronic engineering by modifying the surface adsorption energy may also be accomplished by the anionic exchange.…”
Section: Introductionmentioning
confidence: 99%
“…In analogy to Pt 1 -Ti 1−x O 2 , the z-axis d orbitals of Co(Ti) dominate the contribution to the d-d hybridization (Figures 4c and 4d and Supporting Information Figure S13), which is quite consistent with the proposed atom-realm (AR) effect. 17,33,34 However, one order of magnitude smaller ICOHP indicates much weaker d-d interaction in Co 1 -Ti 1−x O 2 . This is quite consistent with the XPS analysis (Supporting Information Figure S14), in which the binding energy of Ti in Pt 1 -Ti 1−x O 2 shifts to a lower range compared with that of Co 1 -Ti 1−x O 2 , indicating the enhanced charge transfer from Pt to Ti, namely the activation of Ti.…”
Section: Resultsmentioning
confidence: 99%
“…4,5 The pioneering works provide significant inspiration for the geometric and electronic structure regulation on catalysts. [6][7][8][9][10][11][12][13][14][15][16][17][18][19][20] The geometric optimizations focus on tailoring crystal facets, 6,7 refining surface strain, [8][9][10][11] or downgrading into single-atom scale, [12][13][14] while electronic-structure optimization pursues the regulation of charge transfer or d-band center. [15][16][17][18][19][20] However, rational catalyst design via the regulation of d-orbital energies/ orientations has been rarely reported, which requires a comprehensive understanding of the effects of each d orbital on catalysis (Figure 1a).…”
Section: Introductionmentioning
confidence: 99%
“…Noticeably, some new theories such as the atom-realm effect are proposed to guide the synthesis of lattice catalyst, charge catalyst, orbital catalyst and spin catalyst in doped systems. 30 Actually, the in-depth causes of NEGS are that the hybrid orbital of sp 2 carbon atoms is reconstructed, which is discussed in detail below.…”
Section: Resultsmentioning
confidence: 99%