Coupling effects of Zn single atom and high curvature supports for improved performance of CO2 reduction

Hao, Zhongjing; Chen, Junxiang; Zhang, Dafeng; Zheng, Lirong; Li, Yueming; Yin, Zi; He, Gang; Jiao, Lei; Wen, Zhenhai; Lv, Xiaojun

doi:10.1016/j.scib.2021.04.020

Cited by 39 publications

(29 citation statements)

References 57 publications

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“…Single-atom catalysts (SACs) with highly dispersed single metal atoms has demonstrated excellent activity and selectivity for CO 2 RR. − The sp 2 -hybridized carbons, such as graphene, carbon nanotube, and mesoporous carbons, are widely used as SAC supports for CO 2 RR due to its porous structure, tunable chemical properties, and high stability. − It is noted that previous studies on SACs for CO 2 RR have mainly focused on the metal components. 3d transition metals, such as Mn, Fe, Co, Ni, Cu, Zn, are extensively investigated for SACs supported on carbon materials. − The activity and selectivity of SACs are significantly influenced by the center metal atoms, and the intrinsic outer electronic structures of the transition metals play a decisive role. , 25 On the other side, the carbon supports, most of which are sp 2 -hybridized carbons, has been assumably posing a secondary effect, such as providing suitable porosity and electronic conductivity . The innate hybridization of carbon supports for SACs has not been thoroughly investigated.…”

Section: Introductionmentioning

confidence: 99%

Electrochemical CO₂ Reduction Reaction on 3d Transition Metal Single-Atom Catalysts Supported on Graphdiyne: A DFT Study

2021

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In the electrochemical CO2 reduction reaction (CO2RR), single atom catalysts (SACs) supported on carbon materials have exhibited high activity and selectivity. However, the carbon supports are mainly graphene and carbon nanotubes, which are composed of sp2-hybridized carbon. Graphdiyne with sp-hybridization has been investigated as a promising carbon material for various catalytic reactions. In this study, the effect of sp-hybridization on graphdiyne was investigated using density functional theoretical (DFT) calculations for the CO2RR reactivity of Mn, Fe, Co, Ni, Cu, and Zn SACs supported on graphdiyne (M–graphdiyne). Among them, Co–graphdiyne exhibits a high activity and selectivity for CH3OH product, with remarkably low free energy barrier of 0.31 eV, which is superior to SACs supported on graphene with sp2-hybridization. The d-band center and atomic number of the metal atom, and the charge redistribution on sp-hybridization exert significant influence to the energy of intermediates, which are key to understanding the activity and selectivity of SACs in CO2RR.

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Section: Introductionmentioning

confidence: 99%

Electrochemical CO₂ Reduction Reaction on 3d Transition Metal Single-Atom Catalysts Supported on Graphdiyne: A DFT Study

2021

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“…Figure 3D shows that its Zn K-edge XANES edge falls between the Zn foil and ZnO, close to the edge of ZnPc, indicating that the average valence of Zn in NiZn-NC-950 is close to that of ZnPc. 55 The main peak of the Zn K-edge FT-EXAFS spectrum of NiZn-NC-950 is located at 1.50 Å (Figure 3E), which is very close to that of Zn-N in ZnPc (1.58 Å), while the nearby peak located at 1.90 Å can be attributed to the Zn-O path. The small peak at 2.40 Å can be interpreted as a Zn-Ni bond because of its length approaching that in the Zn-Zn foil (2.30 Å), confirming once again the existence of a strong electronic interaction between Ni and Zn.…”

Section: Coordination Structure Of Nizn-nc-950mentioning

confidence: 69%

Boosting the Ni–Zn interplay via O/N dual coordination for high‐efficiency CO₂ electroreduction

et al. 2023

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Design of supportive atomic sites with a controllably adjusted coordinating environment is essential to advancing the reduction of CO2 to value‐added fuels and chemicals and to achieving carbon neutralization. Herein, atomic Ni (Zn) sites that are uniquely coordinated with ternary Zn (Ni)/N/O ligands were successfully decorated on formamide‐derived porous carbon nanomaterials, possibly forming an atomic structure of Ni(N2O1)‐Zn(N2O1), as studied by combining X‐ray photoelectron spectroscopy and X‐ray absorption spectroscopy. With the mediation of additional O coordination, the Ni–Zn dual site induces significantly decreased desorption of molecular CO. The NiZn‐NC decorated with rich Ni(N2O1)‐Zn(N2O1) sites remarkably gained >97% CO Faraday efficiency over a wide potential range of ‒0.8 to ‒1.1 V (relative to reversible hydrogen electrode). Density functional theory computations suggest that the N/O dual coordination effectively modulates the electronic structure of the Ni–Zn duplex and optimizes the adsorption and conversion properties of CO2 and subsequent intermediates. Different from the conventional pathway of using Ni as the active site in the Ni–Zn duplex, it is found that the Ni‐neighboring Zn sites in the Ni(N2O1)‐Zn(N2O1) coordination showed much lower energy barriers of the CO2 protonation step and the subsequent dehydroxylation step.

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“…In addition to the elements in the d zone, the SACs constructed from the elements in the ds zone (including Cu, Zn, Ag, Au) also showed better electrocatalytic CO 2 reduction to CO performance to a certain extent 68,86–92 …”

Section: Transforming Co2 Into Hydrocarbon Fuelsmentioning

confidence: 99%

“…Based on experimental and DFT simulations, we came to the conclusion that the unique Cu 1 x + and the adjacent Cu 1 0 structure in Cu–APC could be easily used for adsorption of H 2 O and CO 2 , respectively, which contributed to enhanced CO 2 conversion. Hao et al 87 reported the synthesis of N‐doped carbon nano‐onion‐supported single‐atom Zn species (named as ZnN/CNO). The results of HAADF‐STEM images and XAFS confirmed that single‐atom Zn was atomically dispersed in ZnN/CNO.…”

Section: Transforming Co2 Into Hydrocarbon Fuelsmentioning

confidence: 99%

Single‐atom catalysis for carbon neutrality

Wang

2022

Carbon Energy

140

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Currently, more than 86% of global energy consumption is still mainly dependent on traditional fossil fuels, which causes resource scarcity and even emission of high amounts of carbon dioxide (CO 2 ), resulting in a severe "Greenhouse effect." Considering this situation, the concept of "carbon neutrality" has been put forward by 125 countries one after another. To achieve the goals of "carbon neutrality," two main strategies to reduce CO 2 emissions and develop sustainable clean energy can be adopted. Notably, these are crucial for the synthesis of advanced single-atom catalysts (SACs) for energyrelated applications. In this review, we highlight unique SACs for conversion of CO 2 into high-efficiency carbon energy, for example, through photocatalytic, electrocatalytic, and thermal catalytic hydrogenation technologies, to convert CO 2 into hydrocarbon fuels (CO, CH 4 , HCOOH, CH 3 OH, and multicarbon [C 2+ ] products). In addition, we introduce advanced energy conversion technologies and devices to replace traditional polluting fossil fuels, such as photocatalytic and electrocatalytic water splitting to produce hydrogen energy and a high-efficiency oxygen reduction reaction (ORR) for fuel cells. Impressively, several representative examples of SACs (including d-, ds-, p-, and f-blocks) for CO 2 conversion, water splitting to H 2 , and ORR are discussed to describe synthesis methods, characterization, and corresponding catalytic activity. Finally, this review concludes with a description of the challenges and outlooks for future applications of SACs in contributing toward carbon neutrality.carbon neutrality, CO 2 reduction reaction, single-atom catalysts, sustainable clean energy | INTRODUCTIONRapid global industrial revolution with increasing combustion of fossil fuels has led to a substantial increase in greenhouse gas emissions, and the Earth's ecological environment is being irreversibly damaged. In fact, the concentration of carbon dioxide (CO 2 ) has increased drastically in the atmosphere from around 280 ppm (in the early 1800s) to 410 ppm (currently). This has led to a drastic increase in global temperatures and corresponding sea-level rise, as shown in Figure 1. 1 Furthermore, this has also led to disruption in the balance of the carbon cycle. As early as 1960, Syukuro Manabe identified this serious problem and established

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Coupling effects of Zn single atom and high curvature supports for improved performance of CO2 reduction

Cited by 39 publications

References 57 publications

Electrochemical CO₂ Reduction Reaction on 3d Transition Metal Single-Atom Catalysts Supported on Graphdiyne: A DFT Study

Electrochemical CO₂ Reduction Reaction on 3d Transition Metal Single-Atom Catalysts Supported on Graphdiyne: A DFT Study

Boosting the Ni–Zn interplay via O/N dual coordination for high‐efficiency CO₂ electroreduction

Single‐atom catalysis for carbon neutrality

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Coupling effects of Zn single atom and high curvature supports for improved performance of CO2 reduction

Cited by 39 publications

References 57 publications

Electrochemical CO2 Reduction Reaction on 3d Transition Metal Single-Atom Catalysts Supported on Graphdiyne: A DFT Study

Electrochemical CO2 Reduction Reaction on 3d Transition Metal Single-Atom Catalysts Supported on Graphdiyne: A DFT Study

Boosting the Ni–Zn interplay via O/N dual coordination for high‐efficiency CO2 electroreduction

Single‐atom catalysis for carbon neutrality

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Electrochemical CO₂ Reduction Reaction on 3d Transition Metal Single-Atom Catalysts Supported on Graphdiyne: A DFT Study

Electrochemical CO₂ Reduction Reaction on 3d Transition Metal Single-Atom Catalysts Supported on Graphdiyne: A DFT Study

Boosting the Ni–Zn interplay via O/N dual coordination for high‐efficiency CO₂ electroreduction