Isolated Ni single atoms in graphene nanosheets for high-performance CO<sub>2</sub> reduction

Jiang, Kun; Siahrostami, Samira; Zheng, Tingting; Hu, Yongfeng; Hwang, Sooyeon; Stavitski, Eli; Peng, Yande; Dynes, James J.; Gangisetty, Mehash; Su, Dong; Attenkofer, Klaus; Wang, Haotian

doi:10.1039/c7ee03245e

Cited by 891 publications

(675 citation statements)

References 62 publications

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“…In the former case,s ubstituted Co phthalocyanine with 8c yano groups led to 5.6 mA cm À2 at 340 mV overpotential (TOF 1.4 s À1 )a nd 88 %C Os electivity,w hile an optimized CO selectivity of 98 %( TOFo f4 .1 s À1 )w as obtained at 520 mV overpotential with ac atalyst loading more than 5t imes larger than ours (Table 2, entry 4, CoPc-CN). Moreover,[Co(qpy)] 2+ also closely matches some of the most active solid electrocatalysts,i ncluding noble metals.A recent class of emerging catalytic materials is given by graphene type materials with atomically dispersed metal atoms,i ncluding notably Ni [21,22] and Co. [23] With cobalt, CO selectivity up to 94 %w as obtained at 520 mV overpotential (TOF 5s À1 )w ith ac urrent density of 18 mA cm À2 ,w hile comparable performances were recently achieved using nickel with selectivity in the range of 95 %a nd current density from 10 to 22 mA cm À2 (TOF from 4.1 to 6.8 s À1 )a t overpotential close to 600 mV.R egarding noble metals, nanostructured silver catalyst can achieve 9mAcm À2 (90 % selectivity) at 390 mV overpotential. [24] Oxide-derived Au nanoparticles can furnish 10 mA cm À2 at only 260 mV overpotential, [25] while state-of-the art gold nanoneedles give aCO current up to 22 mA cm À2 at only 240 mV overpotential ( Table 2, entry 6).…”

Section: Angewandte Chemiementioning

confidence: 99%

A Hybrid Co Quaterpyridine Complex/Carbon Nanotube Catalytic Material for CO₂ Reduction in Water

et al. 2018

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Associating a metal-based catalyst to a carbon-based nanomaterial is a promising approach for the production of solar fuels from CO . Upon appending a Co quaterpyridine complex [Co(qpy)] at the surface of multi-walled carbon nanotubes, CO conversion into CO was realized in water at pH 7.3 with 100 % catalytic selectivity and 100 % Faradaic efficiency, at low catalyst loading and reduced overpotential. A current density of 0.94 mA cm was reached at -0.35 V vs. RHE (240 mV overpotential), and 9.3 mA cm could be sustained for hours at only 340 mV overpotential with excellent catalyst stability (89 095 catalytic cycles in 4.5 h), while 19.9 mA cm was met at 440 mV overpotential. Such a hybrid material combines the high selectivity of a homogeneous molecular catalyst to the robustness of a heterogeneous material. Catalytic performances compare well with those of noble-metal-based nano-electrocatalysts and atomically dispersed metal atoms in carbon matrices.

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Section: Angewandte Chemiementioning

confidence: 99%

A Hybrid Co Quaterpyridine Complex/Carbon Nanotube Catalytic Material for CO₂ Reduction in Water

et al. 2018

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“…There are two characteristic peaks located at 1345 cm −1 (D-band) and 1585 cm −1 (G-band) which, respectively, are the bands of disordered or defective graphite and crystalline graphite. [26,34,39] It is worth mentioning that the I D /I G ratios of Al 2 O 3 /PGM-5 (1.12) and Al 2 O 3 /PGM-12 (1.11) are similar, suggesting that the excess Al 2 O 3 produces only a small increase in defect deactivating. As shown in Figure 1d, the I D /I G ratio of PGM-T is 1.25, apparently higher than for all Al 2 O 3 /PGM hybrids.…”

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confidence: 92%

Deactivating Defects in Graphenes with Al₂O₃ Nanoclusters to Produce Long‐Life and High‐Rate Sodium‐Ion Batteries

Lin

Zhang

Kong

et al. 2018

Advanced Energy Materials

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LIBs), delivers very limited reversible capacity in SIBs due to its inability to form stable low-stage graphite intercalation compounds (GICs). [4,5] Thus, most research has turned to nongraphitic carbons including nanocarbons and hard carbons, [6][7][8][9][10] whose capacities are significantly higher than graphite. It has been found that the structure could be well controlled to realize the high efficiency and reversibility. Our group has reported that the commercial carbon molecular sieves with abundant ultrasmall (0.3-0.5 nm) pores can achieve high efficiency and reversible capacity. [11] Intensive researches have also revealed that the nongraphitic carbons with low specific surface areas (SSA) exhibit a high electrochemical stability. [12][13][14][15][16] However, these carbons show limited rate capability and relatively low capacity. Thus, it is desired to improve the SSA to enhance the rate performance and capacity. Unfortunately, nongraphitic carbons with large SSA and a large number of defects typically exhibit an extremely low initial Coulombic efficiency (ICE) and unsatisfactory cyclic stability because of uncontrollable electrolyte decomposition and ineffective formation of a solid electrolyte interphase (SEI). In a previous report, we used reduced graphene oxide (rGO) as a model anode and found that an ether-based electrolyte can greatly suppress the Carbon materials are the most promising anodes for sodium-ion batteries (SIBs), but low initial Coulombic efficiency (ICE) and poor cyclic stability hinder their practical use. It is shown herein, that an effective but simple remedy for these problems can be achieved by deactivating defects in the carbon with Al 2 O 3 nanocluster coverage. A 3D porous graphene monolith (PGM) is used as the model material and Al 2 O 3 nanoclusters around 1 nm are grown on the defects of graphene. It is shown that these Al 2 O 3 nanoclusters suppress the decomposition of conductive sodium salt in the electrolyte, resulting in the formation of a thin and homogenous solid electrolyte interphase (SEI). In addition, Al 2 O 3 nanoclusters appear to reduce the detrimental etching of the SEI by hydrogen fluoride (HF) and improve its stability. Therefore, after the introduction of Al 2 O 3 nanoclusters, the ICE, cyclic stability, and rate capability of the PGM are greatly improved. A higher ICE (70.2%) and capacity retention (82.9% after 500 cycles at 0.5 A g −1 ) than those of normally reported for large surface area carbons are achieved. This work indicates a new way to deactivate defects and modify the SEI of carbon materials, and hopefully accelerate the commercialization of carbon materials as anode materials for SIBs.

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“…Additionally, the atomic‐scale morphology supplies higher specific surface area exposed to reactants relative to NPs, which crucially affects the density of catalytic active sites. IV) Low coordination number: the high catalytic activity is usually associated with the confined and unsaturated coordination environments of SACs, where the low coordination number gives a flexible degree of shift to ameliorate the catalytic performance . Moreover, the donor number of a few neighboring atoms can be efficiently adjusted to tune the binding energies between the intermediates and active sites, thus changing the product selectivity …”

Section: Introductionmentioning

confidence: 99%

Carbon‐Rich Nonprecious Metal Single Atom Electrocatalysts for CO₂ Reduction and Hydrogen Evolution

et al. 2019

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Single atom catalysts (SACs) are considered as the emerging catalysts for boosting electricity‐driven CO2 reduction reaction (CRR) and hydrogen evolution reaction (HER). To replace the rare and expensive noble metal electrocatalysts, developing nonprecious metal SACs (NPMSACs) with superior electrocatalytic activity and stability is of paramount importance for achieving high efficiency in CRR and HER. Herein, a brief overview of recent achievements in the carbon‐rich NPMSACs for both CRR and HER is provided. The synthesis strategies and corresponding electrocatalytic performances of various carbon‐rich NPMSACs are discussed in the order of various metals (Ni, Co, Fe, Zn, and Sn for CRR, as well as Ni, Co, Fe, Mo, and W for HER), with a special attention paid to understand the structure–activity relationships. Finally, the remaining challenges and future perspectives for enhancing CRR and HER performance of NPMSACs are outlined.

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Isolated Ni single atoms in graphene nanosheets for high-performance CO₂ reduction

Abstract: High-performance electrocatalytic CO2 reduction to CO using Ni single-atom catalyst in an anion membrane electrode assembly.

Cited by 891 publications

References 62 publications

A Hybrid Co Quaterpyridine Complex/Carbon Nanotube Catalytic Material for CO₂ Reduction in Water

A Hybrid Co Quaterpyridine Complex/Carbon Nanotube Catalytic Material for CO₂ Reduction in Water

Deactivating Defects in Graphenes with Al₂O₃ Nanoclusters to Produce Long‐Life and High‐Rate Sodium‐Ion Batteries

Carbon‐Rich Nonprecious Metal Single Atom Electrocatalysts for CO₂ Reduction and Hydrogen Evolution

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Isolated Ni single atoms in graphene nanosheets for high-performance CO2 reduction

Abstract: High-performance electrocatalytic CO2 reduction to CO using Ni single-atom catalyst in an anion membrane electrode assembly.

Cited by 891 publications

References 62 publications

A Hybrid Co Quaterpyridine Complex/Carbon Nanotube Catalytic Material for CO2 Reduction in Water

A Hybrid Co Quaterpyridine Complex/Carbon Nanotube Catalytic Material for CO2 Reduction in Water

Deactivating Defects in Graphenes with Al2O3 Nanoclusters to Produce Long‐Life and High‐Rate Sodium‐Ion Batteries

Carbon‐Rich Nonprecious Metal Single Atom Electrocatalysts for CO2 Reduction and Hydrogen Evolution

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Isolated Ni single atoms in graphene nanosheets for high-performance CO₂ reduction

A Hybrid Co Quaterpyridine Complex/Carbon Nanotube Catalytic Material for CO₂ Reduction in Water

A Hybrid Co Quaterpyridine Complex/Carbon Nanotube Catalytic Material for CO₂ Reduction in Water

Deactivating Defects in Graphenes with Al₂O₃ Nanoclusters to Produce Long‐Life and High‐Rate Sodium‐Ion Batteries

Carbon‐Rich Nonprecious Metal Single Atom Electrocatalysts for CO₂ Reduction and Hydrogen Evolution