Ionic Exchange of Metal−Organic Frameworks for Constructing Unsaturated Copper Single‐Atom Catalysts for Boosting Oxygen Reduction Reaction

Ma, Shenghua; Han, Zheng; Leng, Kunyue; Liu, Xiaojie; Wang, Yi; Qu, Yunteng; Bai, Junhong

doi:10.1002/smll.202001384

Cited by 86 publications

(105 citation statements)

References 31 publications

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“…Bright dots attributed to Cu atoms were clearly observable on the carbon nanosheets of Cu-N-C-800, confirming the successful synthesis of single Cu atoms anchored on the carbon matrix as previously shown. [28] As illustrated in Figure S2a-c (Supporting Information), the Cu-N-C-700 exhibited a similar nanosheet structure and the C, N, and Cu atoms were also detected in it. However, there were no visible bright dots in the (AC) HADDF-STEM image, possibly because the single Cu atoms were covered by the thick carbon nanosheets.…”

Section: Structural Characterizations Of Catalystsmentioning

confidence: 83%

Single‐Atom Cu Catalysts for Enhanced Electrocatalytic Nitrate Reduction with Significant Alleviation of Nitrite Production

Zhu

Chen

Liao

et al. 2020

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237

189

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Metallic Cu is a well-known electrocatalyst for nitrate reduction reaction (NO 3 RR), but it suffers from relatively low activity, poor stability, and inducing nitrite accumulation during the long-term operation. Herein, it is found that Cu catalysts minimized at the single-atom level can overcome the limitations of bulk materials in NO 3 RR. A metal-nitrogen-carbon (M-N-C) electrocatalyst composed of carbon nanosheets embedding isolated copper atoms coordinated with N, Cu-N-C-800, is synthesized by pyrolysis of a Cu-based metal-organic framework at 800 °C. In comparison with Cu nanoparticles and Cu plate-800, kinetic measurements show that the Cu-N-C-800 electrocatalyst is more active and stable and distinctly suppresses the release of nitrite intermediate into the solution. The combined results of experimental data and density functional theory calculations indicate that Cu bound with N (particularly Cu-N 2) is the key to favorable adsorption of NO 3 − and NO 2 −. This strong binding is responsible for the enhanced rate of nitrate conversion to the end products of ammonia and nitrogen. These findings highlight the promise of single-atom Cu electrocatalysts for nitrate reduction with desirable performance.

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Section: Structural Characterizations Of Catalystsmentioning

confidence: 83%

Single‐Atom Cu Catalysts for Enhanced Electrocatalytic Nitrate Reduction with Significant Alleviation of Nitrite Production

Zhu

Chen

Liao

et al. 2020

Small

237

189

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“…For example, Ma et al first synthesized Cu/Zn-ZIF, and then obtained CuN 4 by calcinating the precursor at 800 °C, while CuN 3 was formed at 900 °C. [73] Wang et al also claimed that Co-N 4 , Co-N 3 , and Co-N 2 could be prepared at 800, 900, and 1000 °C, respectively. [74]…”

Section: High-temperature Pyrolysis Methodsmentioning

confidence: 99%

“…synthesized Cu–N 3 by calcinating the precursor at 900 °C, while Cu–N 4 was obtained by calcinating at 800 °C, and reported that Cu–N 3 SAC had a higher half‐wave potential (180 mV higher) and ten times more turnover frequency than that of CuN 4 in 0.1 m KOH solution. [ 73 ] DFT calculations revealed that the energy barrier of O 2 adsorption, the rate‐determining step, for Cu–N 3 (0.17 eV; Figure 5d) was much lower than that for Cu–N 4 (0.87 eV; Figure 5a). For those single metal atomic sites with strong O* adsorption, increasing coordination number could reduce the intermediates adsorption energy and thus promote the catalytic activity.…”

Section: Strategies To Tune the Surrounding Environment Of Atomic Metmentioning

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

272

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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“…For example, Ma et al prepared atomically dispersed copper catalysts with controllable coordination structures. [84] In this process, the adsorbed Cu ions exchange with the Zn nodes in ZIF-8 at high temperature, and then, Cu atoms are trapped in the cavities of the MOFs to form Cu SACs. Notably, changing the pyrolysis temperature can effectively control the structure of the active metal center at the atomic level.…”

Section: Sacsmentioning

confidence: 99%

Which is Better for Nanomedicines: Nanocatalysts or Single‐Atom Catalysts?

Zhao

Zhang

Yang

et al. 2020

Adv Healthcare Materials

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With the rapid advancements in nanotechnology and materials science, numerous nanomaterials have been used as catalysts for nanomedical applications. Their design and modification according to the microenvironment of diseases have been shown to achieve effective treatment. Chemists are in pursuit of nanocatalysts that are more efficient, controllable, and less toxic by developing innovative synthetic technologies and improving existing ones. Recently, single-atom catalysts (SACs) with excellent catalytic activity and high selectivity have attracted increasing attention because of their accurate design as nanomaterials at the atomic level, thereby highlighting their potential for nanomedical applications. In this review, the recent advances in nanocatalysts and SACs are briefly summarized according to their synthesis, characterizations, catalytic mechanisms, and nanomedical applications. The opportunities and future scope for their development and the issues and challenges for their application as nanomedicine are also discussed. As far as it is known, the review is the systematic comparison of nanocatalysts and SACs, especially in the field of nanomedicine, which has promoted the development of nanocatalytic medicine.

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Ionic Exchange of Metal−Organic Frameworks for Constructing Unsaturated Copper Single‐Atom Catalysts for Boosting Oxygen Reduction Reaction

Cited by 86 publications

References 31 publications

Single‐Atom Cu Catalysts for Enhanced Electrocatalytic Nitrate Reduction with Significant Alleviation of Nitrite Production

Single‐Atom Cu Catalysts for Enhanced Electrocatalytic Nitrate Reduction with Significant Alleviation of Nitrite Production

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

Which is Better for Nanomedicines: Nanocatalysts or Single‐Atom Catalysts?

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