Single-Ni-atom catalyzes aqueous phase electrochemical reductive dechlorination reaction

Xu, Yongfu; Yao, Zeqing; Mao, Zhechuan; Shi, Meiqin; Zhang, Xiaoyong; Cheng, Feng; Yang, Hong Bin; Tao, Hua Bing; Liu, Bin

doi:10.1016/j.apcatb.2020.119057

Cited by 60 publications

(25 citation statements)

References 57 publications

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“…Liu's group has made great efforts to minimize the gap between measured catalytic activity and theoretical result. [ 150–153 ] For example, Gao et al. performed kinetic analysis to experimentally probe the rate‐determining step in ORR and found that the reaction rate of H + in the rate‐determining step was −0.05 to −0.07, very close to 0.…”

Section: Discussionmentioning

confidence: 99%

“…Liu's group has made great efforts to minimize the gap between measured catalytic activity and theoretical result. [150][151][152][153] For example, Gao et al performed kinetic analysis to experimentally probe the rate-determining step in ORR and found that the reaction rate of H + in the rate-determining step was −0.05 to −0.07, very close to 0. [94] Therefore, it was suggested that H + was not involved in the rate-limiting step in ORR and it was deduced that the ratedetermining step of producing H 2 O 2 over Co-NC is as follows:…”

Section: Discussionmentioning

confidence: 99%

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Coordination Engineering of Single‐Atom Catalysts for the Oxygen Reduction Reaction: A Review

Zhang

Yang

Liu

2020

Advanced Energy Materials

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278

185

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Future renewable energy supplies and a sustainable environment rely on many important catalytic processes. Single‐atom catalysts (SACs) are attractive because of their maximum atom utilization efficiency, tunable electronic structures, and outstanding catalytic performance. Of particular note, transition‐metal SACs exhibit excellent catalytic activity and selectivity for the oxygen reduction reaction (ORR)—an important half reaction in fuel cells and metal–air batteries as well as for portable hydrogen peroxide (H2O2) production. Although considerable efforts have been made on the synthesis of SACs for ORR, the regulation of the coordination environments of SACs and thus the electronic structures still pose a big challenge. In this review, strategies for manipulating the coordination environments of SACs are classified into three categories, including regulation of the center metal atoms, manipulation of the surrounding environment connecting to the center metal atom, and modification of the geometric configuration of the support. Finally, some issues regarding the future development of SACs for ORR are raised and possible solutions are proposed.

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Section: Discussionmentioning

confidence: 99%

Section: Discussionmentioning

confidence: 99%

Coordination Engineering of Single‐Atom Catalysts for the Oxygen Reduction Reaction: A Review

Zhang

Yang

Liu

2020

Advanced Energy Materials

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278

185

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“…Nickel-based single-atom catalysts have been employed in many reactions. The most prominent examples include the electrocatalytic HER, ,,,, OER, ,, ORR, and CO 2 RR,. ,,,,− Other applications comprise the electrochemical dechlorination of chlorinated organic pollutatants, methanol oxidation, and ethanol oxidation, lithium–sulfur batteries, dye-sensitized solar cells, photocatalytic reduction of CO 2 and hydrogen evolution reaction, photothermal CO 2 methanation, reverse water–gas shift reaction, dry reforming of CH 4 , , oxidations of benzene, oxidative esterification of primary alcohols, dehydrogenation of ethanol , and alkanes, selective hydrogenations of acetylene, nitroarenes, olefins, and various unsaturated substrates, and cellulose valorization …”

Section: Late Transition Metalsmentioning

confidence: 99%

“…The most prominent examples include the electrocatalytic HER, 264,362,372,382,386 OER, 38,364,381 ORR, 42 and CO 2 RR,. 43,138,363,377,391−393 Other applications comprise the electrochemical dechlorination of chlorinated organic pollutatants, 394 methanol oxidation, 372 and ethanol oxidation, 372 lithium−sulfur batteries, 389 dye-sensitized solar cells, 228 photocatalytic reduction of CO 2 384 and hydrogen evolution reaction, 395 photothermal CO 2 methanation, 365 reverse water−gas shift reaction, 366 dry reforming of CH 4 , 367,385 oxidations of benzene, 309 oxidative esterification of primary alcohols, 293 dehydrogenation of ethanol 369,370 and alkanes, 375 selective hydrogenations of acetylene, 368 nitroarenes, 396 olefins, 373 and various unsaturated substrates, 388 and cellulose valorization. 388 In the electrocatalytic CO 2 reduction reaction, Ni single atoms supported on N-doped CNTs and graphene oxides outperform the Ni nanoparticles in terms of onset potential, current density, and CO Faradaic efficiency.…”

Section: Coordination Environment and Electronic Properties Nickel-ba...mentioning

confidence: 99%

Single-Atom Catalysts across the Periodic Table

et al. 2020

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Isolated atoms featuring unique reactivity are at the heart of enzymatic and homogeneous catalysts. In contrast, although the concept has long existed, single-atom heterogeneous catalysts (SACs) have only recently gained prominence. Host materials have similar functions to ligands in homogeneous catalysts, determining the stability, local environment, and electronic properties of isolated atoms and thus providing a platform for tailoring heterogeneous catalysts for targeted applications. Within just a decade, we have witnessed many examples of SACs both disrupting diverse fields of heterogeneous catalysis with their distinctive reactivity and substantially enriching our understanding of molecular processes on surfaces. To date, the term SAC mostly refers to late transition metal-based systems, but numerous examples exist in which isolated atoms of other elements play key catalytic roles. This review provides a compositional encyclopedia of SACs, celebrating the 10th anniversary of the introduction of this term. By defining single-atom catalysis in the broadest sense, we explore the full elemental diversity, joining different areas across the whole periodic table, and discussing historical milestones and recent developments. In particular, we examine the coordination structures and associated properties accessed through distinct single-atom−host combinations and relate them to their main applications in thermo-, electro-, and photocatalysis, revealing trends in element-specific evolution, host design, and uses. Finally, we highlight frontiers in the field, including multimetallic SACs, atom proximity control, and possible applications for multistep and cascade reactions, identifying challenges, and propose directions for future development in this flourishing field.

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“…More importantly, both Ni and Fe showed zero valence, which was different from other Ni-or Fe-based SACs with positive valence states or mixed valence states using graphene as the support. 104,105 These researchers found that Ni/Fe atoms have a strong chemical interaction and electronic coupling with GDY according to theoretical calculations, which not only favored the stabilization of Ni/Fe atoms on the GDY, but also accelerated charge transport (Fig. 2A).…”

Section: Hydrogen Evolution Reactionmentioning

confidence: 94%