Charge Polarization from Atomic Metals on Adjacent Graphitic Layers for Enhancing the Hydrogen Evolution Reaction

Abstract

Atomic metal species-based catalysts (AMCs) show remarkable possibilities in various catalytic reactions.T he coordination configuration of the metal atoms has been widely recognized as the determining factor to the electronic structure and the catalytic activity.H owever,t he synergistic effect between the adjacent layers of the multilayered AMCs is always neglected. We reported an atomic Co and Pt co-trapped carbon catalyst, whichexhibits aultrahigh activity for HER in the wide range of pH (h 10 = 27 and 50 mV in acidic and alkaline media, respectively) with ultralow metal loadings (1.72 and 0.16 wt %f or Co and Pt, respectively), which is much superior to the commercial Pt/C.T heoretical analysis reveals that the atomic metals on the inner graphitic layers significantly alter the electronic structure of the outmost layer,thus tailoring the HER activity.T his finding arouses ar e-thinking of the intrinsic activity origins of AMCs and suggests anew avenue in the structure design of AMCs.

Engineering Local Coordination Environments of Atomically Dispersed and Heteroatom‐Coordinated Single Metal Site Electrocatalysts for Clean Energy‐Conversion

“…m) Free energy profile and n) LSV for both A‐CoPt‐NG and A‐CoPt‐MNG catalysts in both acidic and alkaline solutions. Reproduced with permission . Copyright 2019, Wiley‐VCH.…”

“…Construction of dual‐metal sites is a promising way to modify the local electronic structure of SACs. A Co–Pt dual‐metal site on hollow multilayered carbon shells (A‐CoPt‐NC) was synthesized by pyrolysis of Co‐based MOFs followed by electrodeposition of Pt atoms . The STEM images and XAS spectra indicate that the Co–Pt sites were stabilized by eight N atoms and four C atoms to form two adjacent pyridine‐type MN 4 configurations.…”

“…These sites usually exhibit synergistic effects. Several dual metal sites have demonstrated their superiority in energy‐related electrocatalysis including N‐coordinated Co–Fe, Co–Pt, Zn–Co, and Fe–Mn for the ORR, Co–Pt, and Pt–Ru for the HER, and Fe–Ni for the CO 2 RR …”

Partial‐Single‐Atom, Partial‐Nanoparticle Composites Enhance Water Dissociation for Hydrogen Evolution

“…Subsequently, gas chromatography was employed to detect the H 2 production, which shows that the Faradaic efficiency of Ru/Fe–N–C is nearly 100% under a wide range of potentials (Figure 2g; Figure S25, Supporting Information). In terms of η 10 (9 mV) and Tafel slope (28 mV dec −1 ), Ru/Fe–N–C outperforms or is comparable to the state‐of‐the‐art metal‐based HER electrocatalysts including NiFeRu‐LDH (29 mV, 31 mV dec −1 ), [ 40 ] A–CoPt–NC (50 mV, 48 mV dec −1 ), [ 41 ] Ru@C 2 N (17 mV, 38 mV dec −1 ), [ 4 ] Ru 2 P/NPC (52 mV, 69 mV dec −1 ), [ 42 ] Ru@CQDs (10 mV, 47 mV dec −1 ), [ 19 ] RuCo@NC (28 mV, 31 mV dec −1 ), [ 14 ] Ru@CN (32 mV, 53 mV dec −1 ), [ 17 ] RuSAs + RuNPs@MHC (7 mV, 29 mV dec −1 ), [ 43 ] and Cu/Ru@G N (8 mV, 29 mV dec −1 ) [ 44 ] (Figure 2h; Table S6, Supporting Information). Turnover frequency (TOF) is the most effective figure of merit to characterize intrinsic electrocatalytic activity of catalysts.…”

Ultralow-temperature assisted synthesis of single platinum atoms anchored on carbon nanotubes for efficiently electrocatalytic acidic hydrogen evolution

“…Hydrogen (H 2 ) is one of promising renewable energy source candidates to mitigate the consumption of fossil fuels and related environmental problems, owing to its high energy density and zero-emission fuel when burned with oxygen [1][2][3][4][5][6][7][8] . In the recent years, electrocatalytic water splitting into hydrogen on the catalysts have drawn increasing attentions, since hydrogen evolution reaction (HER) from electrocatalytic water splitting is one of a cost-effective and environmentally friendly technologies to produce hydrogen and enable a clean fuel cycle [9][10][11][12][13][14][15][16][17][18][19][20][21][22][23] .…”