A sulfur-tethering synthesis strategy toward high-loading atomically dispersed noble metal catalysts

Wang, Lei; Chen, Ming‐Xi; Yan, Qiangqiang; Xu, Shilong; Chu, Shengqi; Chen, Ping; Lin, Yue; Liang, Hai‐Wei

doi:10.1126/sciadv.aax6322

Cited by 205 publications

(118 citation statements)

References 47 publications

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“…The metal loading of the M-SA-NSFCs could, again, be controlled by adjusting the relative amounts of metal precursors, yielding M-SA-NSFCs with maximum metal loadings of 12.2, 10.9, 15.7, and 15.6 wt% for Co, Ru, Ir, and Pt, respectively. Again, these values are much higher than those reported in most of the previous publications (SupplementaryTable 1)3,10,29,40 .Electrocatalytic ORR performance of Fe-SA-NSFC. The electrochemical performance of Fe-SA-NSFC for the ORR and the effect of the S and F dopants were studied using rotating disk electrode (RDE) and rotating ring-disk electrode (RRDE) measurements.…”

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confidence: 57%

“…with an optimal dosage. For noble metals, thermal reduction was performed under a H 2 /Ar atmosphere at 250°C for 2 h owing to the high reduction ability of H 2 29 . Similar to the characterization of the Fe-SA-NSFC, the XRD, TEM, HRTEM, elemental mapping, and XPS methods were employed to investigate the crystalline structure, morphology, and element distribution of the obtained M-SA-NSFCs ( Supplementary Fig.…”

Section: Resultsmentioning

confidence: 99%

“…However, the surface free energy of metals increases significantly with decreasing particle size, leading to the successive formation of clusters and nanoparticles with a lower activity 5 . Various concepts have been proposed to fabricate SACs through the stabilization of metal atoms on supports 20,21 , such as defect engineering of metal hydroxide and oxide supports 22 , spatial confinement in zeolites 23,24 , fabrication of metal-organic frameworks (MOFs) or covalent-organic frameworks [25][26][27] , and utilization of strong interactions between metal species and coordinating heteroatoms (e.g., nitrogen (N), oxygen (O), and sulfur (S)) [28][29][30] . For example, Zhang et al 20 demonstrated that defects in nickel hydroxide (Ni(OH) x ) could serve as 'traps' to stabilize metal species, achieving a Pt loading much higher than that attained by using defect-free Ni(OH) x .…”

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confidence: 99%

“…IrN 4 , and PtN 4 , respectively29,40 . The metal loading of the M-SA-NSFCs could, again, be controlled by adjusting the relative amounts of metal precursors, yielding M-SA-NSFCs with maximum metal loadings of 12.2, 10.9, 15.7, and 15.6 wt% for Co, Ru, Ir, and Pt, respectively.…”

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confidence: 99%

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Multilayer stabilization for fabricating high-loading single-atom catalysts

et al. 2020

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Metal single-atom catalysts (M-SACs) have emerged as an attractive concept for promoting heterogeneous reactions, but the synthesis of high-loading M-SACs remains a challenge. Here, we report a multilayer stabilization strategy for constructing M-SACs in nitrogen-, sulfur- and fluorine-co-doped graphitized carbons (M = Fe, Co, Ru, Ir and Pt). Metal precursors are embedded into perfluorotetradecanoic acid multilayers and are further coated with polypyrrole prior to pyrolysis. Aggregation of the metals is thus efficiently inhibited to achieve M-SACs with a high metal loading (~16 wt%). Fe-SAC serves as an efficient oxygen reduction catalyst with half-wave potentials of 0.91 and 0.82 V (versus reversible hydrogen electrode) in alkaline and acid solutions, respectively. Moreover, as an air electrode in zinc–air batteries, Fe-SAC demonstrates a large peak power density of 247.7 mW cm−2 and superior long-term stability. Our versatile method paves an effective way to develop high-loading M-SACs for various applications.

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confidence: 57%

Section: Resultsmentioning

confidence: 99%

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confidence: 99%

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Multilayer stabilization for fabricating high-loading single-atom catalysts

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“…Previously, we have thoroughly summarized the advances of supported noble metal SACs for heterogeneous catalysis (15); however, few reports specified and highlighted the microenvironment engineering of SACs for electrochemical applications. Recently, diverse strategies have been developed for rational design of SACs with well-controlled microenvironments, and numbers of experimental and theoretical efforts have been made aimed at in-depth understanding of the microenvironment-activity relationships and the underlying reaction mechanisms in various electrochemical energy conversion reactions (29)(30)(31)(32)(33)(34)(35)(36)(37).…”

Section: Introductionmentioning

confidence: 99%

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

et al. 2020

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Single-atom catalysts (SACs) have become the most attractive frontier research field in heterogeneous catalysis. Since the atomically dispersed metal atoms are commonly stabilized by ionic/covalent interactions with neighboring atoms, the geometric and electronic structures of SACs depend greatly on their microenvironment, which, in turn, determine the performances in catalytic processes. In this review, we will focus on the recently developed strategies of SAC synthesis, with attention on the microenvironment modulation of single-atom active sites of SACs. Furthermore, experimental and computational advances in understanding such microenvironment in association to the catalytic activity and mechanisms are summarized and exemplified in the electrochemical applications, including the water electrolysis and O2/CO2/N2 reduction reactions. Last, by highlighting the prospects and challenges for microenvironment engineering of SACs, we wish to shed some light on the further development of SACs for electrochemical energy conversion.

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