A copper single-atom catalyst towards efficient and durable oxygen reduction for fuel cells

Cui, Liting; Cui, Lirui; Li, Zheng Jian; Zhang, Jin; Wang, Haining; Lu, Shanfu; Xiang, Yan

doi:10.1039/c9ta03518d

Cited by 162 publications

(119 citation statements)

References 40 publications

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“…In fact, the experimental explanation on active species of Cu-SACs for ORR is still severely dependent on X-ray absorption near-edge structure (XANES) and EXAFS without better techniques. Among them, the carbon-hosted CuN 4 moiety has been proposed to be considered as an active center of Cu-SACs [ 27 – 29 , 31 , 32 ], based on the coordination number (4) of Cu in the microstructure. Nevertheless, with a computational hydrogen electrode (CHE) model, the well-established Cu-SAC model with CuN 4 center possesses rather inferior ORR activity to Pt(111) according to the theoretical onset potential (0.25~0.43 V vs. 0.79 V) [ 27 , 28 , 31 – 33 ], which indicates that the atomic-level understanding on the active center of Cu-SACs boosting ORR remains controversial.…”

Section: Introductionmentioning

confidence: 99%

“…Among them, the carbon-hosted CuN 4 moiety has been proposed to be considered as an active center of Cu-SACs [ 27 – 29 , 31 , 32 ], based on the coordination number (4) of Cu in the microstructure. Nevertheless, with a computational hydrogen electrode (CHE) model, the well-established Cu-SAC model with CuN 4 center possesses rather inferior ORR activity to Pt(111) according to the theoretical onset potential (0.25~0.43 V vs. 0.79 V) [ 27 , 28 , 31 – 33 ], which indicates that the atomic-level understanding on the active center of Cu-SACs boosting ORR remains controversial. More importantly, previous studies demonstrated that numerous catalysts experienced reconstruction during the test operation, probably originating from some physical and chemical aspects, such as pH, potential polarization, and adsorbates [ 34 – 36 ].…”

Section: Introductionmentioning

confidence: 99%

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Oxygen-Reconstituted Active Species of Single-Atom Cu Catalysts for Oxygen Reduction Reaction

Liu

et al. 2020

Research

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Identification of an active center of catalysts under realistic working conditions of oxygen reduction reaction (ORR) still remains a great challenge and unclear. Herein, we synthesize the Cu single atom embedded on nitrogen-doped graphene-like matrix electrocatalyst (abbreviated as SA-Cu/NG). The results show that SA-Cu/NG possesses a higher ORR capability than 20% Pt/C at alkaline solution while the inferior activity to 20% Pt/C at acidic medium. Based on the experiment and simulation calculation, we identify the atomic structure of Cu-N2C2 in SA-Cu/NG and for the first time unravels that the oxygen-reconstituted Cu-N2C2-O structure is really the active species of alkaline ORR, while the oxygen reconstitution does not happen at acidic medium. The finding of oxygen-reconstituted active species of SA-Cu/NG at alkaline media successfully unveils the bottleneck puzzle of why the performance of ORR catalysts at alkaline solution is better than that at acidic media, which provides new physical insight into the development of new ORR catalysts.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Oxygen-Reconstituted Active Species of Single-Atom Cu Catalysts for Oxygen Reduction Reaction

Liu

et al. 2020

Research

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“…Besides Fe and Co SAs, copper (Cu) and zinc (Zn) SAs were also reported to show remarkable electrocatalytic activities. [95][96][97][98][99][100] Similar to the preparation of Fe and Co SAs, the precursor strategy has also been widely employed for preparing Cu and Zn SAs. For instance, abundant Cu SA active sites were prepared through the pyrolysis of Cu-based organic precursors mixed with dicyandiamide.…”

Section: Orrmentioning

confidence: 99%

Emerging Metal Single Atoms in Electrocatalysts and Batteries

Zhu

Wang

et al. 2020

Adv Funct Materials

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Energy conversion and storage applications require highly stable and efficient electrocatalysts/electrodes to facilitate electrochemical reactions, but these materials commonly suffer from serious atom wastes and lower performances than the theoretical levels, which cannot meet the increasing demands of the green atomic economy, thereby limiting their practical applications. Recently, metal single atoms (SAs) have attracted tremendous attention owing to their merits of full atom utilization, unique electronic structures, tunable surface characteristics, and low costs. However, metal SAs usually have relatively low physical/chemical stabilities due to their high surface energy, which results in severe degradation of electrochemical performances. Novel synthetic strategies are developed for metal SAs with better stability and performance. In this review, these strategies will be introduced in the context of electrocatalysis and batteries. Specifically, the design concepts, synthesis approach properties, and applications of metal SAs will be discussed. Finally, the critical challenges and future perspectives of metal SAs are presented. This review aims to provide new insights for future work as well as the real-world applications of metal SAs.

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“…Carbon nanotubes have also been used as a substrate for single‐atom Cu catalyst, for example in 2019 Xiang and co‐workers pyrolyzed Cu phthalocyanine in combination with oxidized carbon nanotubes producing Cu–N x moieties. The observed Cu species were in line with other publications, where Cu + and Cu 2+ forms Cu–N 2 or Cu–N 4 sites.…”

Section: Non‐cobalt‐ or Iron‐based Electrocatalystsmentioning

confidence: 99%

Oxygen Reduction Reactions on Single‐ or Few‐Atom Discrete Active Sites for Heterogeneous Catalysis

Sharifi

Gracia‐Espino

Chen

et al. 2019

Advanced Energy Materials

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The oxygen reduction reaction (ORR) is of great importance in energy‐converting processes such as fuel cells and in metal–air batteries and is vital to facilitate the transition toward a nonfossil dependent society. The ORR has been associated with expensive noble metal catalysts that facilitate the O2 adsorption, dissociation, and subsequent electron transfer. Single‐ or few‐atom motifs based on earth‐abundant transition metals, such as Fe, Co, and Mo, combined with nonmetallic elements, such as P, S, and N, embedded in a carbon‐based matrix represent one of the most promising alternatives. Often these are referred to as single atom catalysts; however, the coordination number of the metal atom as well as the type and nearest neighbor configuration has a strong influence on the function of the active sites, and a more adequate term to describe them is metal‐coordinated motifs. Despite intense research, their function and catalytic mechanism still puzzle researchers. They are not molecular systems with discrete energy states; neither can they fully be described by theories that are adapted for heterogeneous bulk catalysts. Here, recent results on single‐ and few‐atom electrocatalyst motifs are reviewed with an emphasis on reports discussing the function and the mechanism of the active sites.

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A copper single-atom catalyst towards efficient and durable oxygen reduction for fuel cells

Abstract: Cu single-atom catalysts could be promising non-noble catalysts towards oxygen reduction for fuel cell applications.

Cited by 162 publications

References 40 publications

Oxygen-Reconstituted Active Species of Single-Atom Cu Catalysts for Oxygen Reduction Reaction

Oxygen-Reconstituted Active Species of Single-Atom Cu Catalysts for Oxygen Reduction Reaction

Emerging Metal Single Atoms in Electrocatalysts and Batteries

Oxygen Reduction Reactions on Single‐ or Few‐Atom Discrete Active Sites for Heterogeneous Catalysis

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