Enhancing CO<sub>2</sub> Electroreduction with the Metal–Oxide Interface

Gao, Dunfeng; Zhang, Yi; Zhou, Zhiwen; Fan, Caimei; Zhao, Xuebing; Huang, Wugen; Li, Yangsheng; Zhu, Junfa; Liu, Ping; Yang, Fan; Wang, Qianqian; Bao, Xinhe

doi:10.1021/jacs.7b00102

Cited by 535 publications

(392 citation statements)

References 29 publications

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“…These approaches include catalyst nanostructuring [2d, 3] or the use of mixed oxides. [6] To support such concepts,m uch effort has focused on the reaction mechanisms and active species in cobalt oxide OER catalysts through theoretical modeling [7] and in situ spectroscopic techniques. [6] To support such concepts,m uch effort has focused on the reaction mechanisms and active species in cobalt oxide OER catalysts through theoretical modeling [7] and in situ spectroscopic techniques.…”

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confidence: 99%

The Structure of the Cobalt Oxide/Au Catalyst Interface in Electrochemical Water Splitting

et al. 2018

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The catalytic synergy between cobalt oxide and gold leads to strong promotion of the oxygen evolution reaction (OER)-one half-reaction of electrochemical water splitting. However, the mechanism behind the enhancement effect is still not understood, in part due to a missing structural model of the active interface. Using a novel interplay of cyclic voltammetry (CV) for electrochemistry integrated with scanning tunneling microscopy (STM) and X-ray photoelectron spectroscopy (XPS) on an atomically defined cobalt oxide/Au(111) system, we reveal here that the supporting gold substrate uniquely favors a flexible cobalt-oxyhydroxide/Au interface in the electrochemically active potential window and thus suppresses the formation of less active bulk cobalt oxide morphologies. The findings substantiate why optimum catalytic synergy is obtained for oxide coverages on gold close to or below one monolayer, and provide the first morphological description of the active phase during electrocatalysis.

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confidence: 99%

The Structure of the Cobalt Oxide/Au Catalyst Interface in Electrochemical Water Splitting

et al. 2018

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“…Recently, those factors have been extensively maneuvered to modulate the performance in electrocatalytic CO 2 reduction [172][173][174][175]. Due to the theme and length limitation of this review, we will not deeply discuss these matters in this review.…”

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confidence: 99%

Recent progress on advanced design for photoelectrochemical reduction of CO2 to fuels

et al. 2018

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The energy crisis and global warming become severe issues. Solar-driven CO 2 reduction provides a promising route to confront the predicaments, which has received much attention. The photoelectrochemical (PEC) process, which can integrate the merits of both photocatalysis and electrocatalysis, boosts splendid talent for CO 2 reduction with high efficiency and excellent selectivity. Recent several decades have witnessed the overwhelming development of PEC CO 2 reduction. In this review, we attempt to systematically summarize the recent advanced design for PEC CO 2 reduction. On account of basic principles and evaluation parameters, we firstly highlight the subtle construction for photocathodes to enhance the efficiency and selectivity of CO 2 reduction, which includes the strategies for improving light utilization, supplying catalytic active sites and steering reaction pathway. Furthermore, diversiform novel PEC setups are also outlined. These exploited setups endow a bright window to surmount the intrinsic disadvantages of photocathode, showing promising potentials for future applications. Finally, we underline the challenges and key factors for the further development of PEC CO 2 reduction that would enable more efficient designs for setups and deepen systematic understanding for mechanisms.

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“…[20,21] The behavior of the porous single-crystalline Fe 3 N electrode during CO 2 RR is examined under experimental conditions that have been widely used in the literature. However, the ultimate technological viability of CO 2 RR is contingent upon the identification of affordable electrocatalysts that overcome the challenges regarding poor product selectivity, high overpotential, and low durability.…”

Section: Metallic Porous Single Crystalsmentioning

confidence: 99%

Metallic Porous Iron Nitride and Tantalum Nitride Single Crystals with Enhanced Electrocatalysis Performance

Zhang

Lin

et al. 2018

Advanced Materials

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Previous studies show that the metalnitrogen moieties with unsaturated nitrogen coordination numbers possess higher catalytic activities and the reported smallest nitrogen coordination number is confirmed to be ≈2 for Co-N 2 and Fe-N 2 moieties using extended X-ray absorption fine structure spectra analysis. [4][5][6] These results indeed give an in-depth insight at the atomic level into structural dependence of catalytic activity of metal nitride nanoparticles by closely correlating the average structural information with catalytic performances. However, the active metalnitrogen moieties confined at the surface layer of materials that host catalysis reactions still remain unclear.Building metal-nitrogen moieties with unsaturated nitrogen coordination numbers to enhance material's catalytic activity remains a fundamental challenge. The state-of-the-art pyrolysis technique of specific precursors is commonly used to construct metal-nitrogen moieties. However, the simultaneous presence of multiple metal species in most composite catalysts makes it highly complex to understand the nature of metal-nitrogen moieties. [7][8][9][10] The short length scale of nanostructured catalysts makes it extremely challenging to quantify metal-nitrogen moiety structure and distributions and to correspondingly elucidate the electronic structure features and unusual activity. The metal-nitrogen moieties are indeed a kind of active clusters at atomic level, which are strictly confined at lattice in local structures in crystalline composites. The polycrystalline or amorphous states of composites make it highly uncertain to construct resolved metal-nitrogen moieties and to accordingly expose these active centers on material's surfaces to host catalysis reactions. Another consideration should be given to the resolved structural feature and chemical composition of moieties that tailor electronic structures to facilitate catalysis functionalities.Single crystals with porosity, combining the advantages of long-range structural coherence of bulk crystals and large surface areas of porous materials, could provide opportunities to host the metal-nitrogen moieties with unsaturated nitrogen coordination on surface. The long-range structural coherence in single crystals offers the possibility to stabilize the metalnitrogen moieties in lattice of local structures on crystalline surfaces especially on the condition that the surface moieties have similar chemical compositions to bulk crystals. Porous Altering a material's catalytic properties would require identifying structural features that deliver electrochemically active surfaces. Single-crystalline porous materials, combining the advantages of long-range ordering of bulk crystals and large surface areas of porous materials, would create sufficient active surfaces by stabilizing 2D active moieties confined in lattice and may provide an alternative way to create high-energy surfaces for electrocatalysis that are kinetically trapped. Here, a radical concept of building active metalnitrogen moieties ...

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Enhancing CO₂ Electroreduction with the Metal–Oxide Interface

Cited by 535 publications

References 29 publications

The Structure of the Cobalt Oxide/Au Catalyst Interface in Electrochemical Water Splitting

The Structure of the Cobalt Oxide/Au Catalyst Interface in Electrochemical Water Splitting

Recent progress on advanced design for photoelectrochemical reduction of CO2 to fuels

Metallic Porous Iron Nitride and Tantalum Nitride Single Crystals with Enhanced Electrocatalysis Performance

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Enhancing CO2 Electroreduction with the Metal–Oxide Interface

Cited by 535 publications

References 29 publications

The Structure of the Cobalt Oxide/Au Catalyst Interface in Electrochemical Water Splitting

The Structure of the Cobalt Oxide/Au Catalyst Interface in Electrochemical Water Splitting

Recent progress on advanced design for photoelectrochemical reduction of CO2 to fuels

Metallic Porous Iron Nitride and Tantalum Nitride Single Crystals with Enhanced Electrocatalysis Performance

Contact Info

Product

Resources

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Enhancing CO₂ Electroreduction with the Metal–Oxide Interface