Selective Electrochemical H<sub>2</sub>O<sub>2</sub> Production through Two‐Electron Oxygen Electrochemistry

Jiang, Yuanyuan; Ni, Pengjuan; Chen, Chuanxia; Lu, Yizhong; Yang, Ping; Kong, Biao; Fisher, Adrian C.; Wang, Xin

doi:10.1002/aenm.201801909

Cited by 555 publications

(419 citation statements)

References 174 publications

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“…While several typical industrial processes, such as Haber–Bosch process, anthraquinone process, etc., are the main routes to produce the important intermediates and fuels (i.e., H 2 O 2 , HCOOH, and NH 3 ), it still comes with many problems, such as extreme energy dependence, explosion dangers, environmental pollution, limited efficiency, and so on. [ 1–3 ] The electrochemical approach, being milder, cleaner, and more efficient, has emerged as a versatile route for yielding the important chemical intermediates and fuels via these electrochemical conversions. [ 4–8 ] In electro catalysis, while the electrocatalysts play a vital role in reducing the activation energy of the reaction and driving the reaction, developing highly efficient electrocatalysts is of great significance.…”

Section: Figurementioning

confidence: 99%

“…[ 9,10 ] O 2 reduction reaction (ORR) represents an attractive alternative to prepare H 2 O 2 with the feature of environmentally friendly and safe, but electrocatalysts suffer from high cost, limited selectivity, and/or low activity. [ 1,2,11,12 ] Besides H 2 O 2 , HCOOH, an important intermediate in industry and the chemical fuel in direct HCOOH fuel cells, is a common CO 2 reduction reaction (CO 2 RR) product, [ 13–15 ] but developing the active, selective, durable, and cheap electrocatalysts for CO 2 RR is also very challenging. [ 16–21 ] NH 3 , another highly value‐added chemical, is one of the most widely used chemicals because it is a source of N 2 for fertilizer and potential transportation fuel.…”

Section: Figurementioning

confidence: 99%

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Exploring Bi₂Te₃ Nanoplates as Versatile Catalysts for Electrochemical Reduction of Small Molecules

et al. 2020

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The electroreduction of small molecules to high value‐added chemicals is considered as a promising way toward the capture and utilization of atmospheric small molecules. Discovering cheap and efficient electrocatalysts with simultaneously high activity, selectivity, durability, and even universality is desirable yet challenging. Herein, it is demonstrated that Bi2Te3 nanoplates (NPs), cheap and noble‐metal‐free electrocatalysts, can be adopted as highly universal and robust electrocatalysts, which can efficiently reduce small molecules (O2, CO2, and N2) into targeted products simultaneously. They can achieve excellent activity, selectivity and durability for the oxygen reduction reaction with almost 100% H2O2 selectivity, the CO2 reduction reaction with up to 90% Faradaic efficiency (FE) of HCOOH, and the nitrogen reduction reaction with 7.9% FE of NH3. After electrochemical activation, an obvious Te dissolution happens on the Bi2Te3 NPs, creating lots of Te vacancies in the activated Bi2Te3 NPs. Theoretical calculations reveal that the Te vacancies can modulate the electronic structures of Bi and Te. Such a highly electroactive surface with a strong preference in supplying electrons for the universal reduction reactions improves the electrocatalytic performance of Bi2Te3. The work demonstrates a new class of cheap and versatile catalysts for the electrochemical reduction of small molecules with potential practical applications.

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Section: Figurementioning

confidence: 99%

Section: Figurementioning

confidence: 99%

Exploring Bi₂Te₃ Nanoplates as Versatile Catalysts for Electrochemical Reduction of Small Molecules

et al. 2020

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“…However, from a chemical production viewpoint, the 2e‐ORR provides the simplest way to generate H 2 O 2 . The use of the 2e‐ORR to generate H 2 O 2 is a newly emerging direction of electrocatalysis . As such, many key issues regarding the design and development of high‐performance 2e‐ORR electrocatalysts remain largely unexplored, offering rich opportunities for researchers in the field.…”

Section: Emerging Applications In the Electrocatalytic Conversion Of mentioning

confidence: 99%

“…To date, the study of electrocatalytic O 2 reductions has been focused on the conversion of O 2 to H 2 O through a 4e‐ORR process . Fortunately, the importance of the 2e‐ORR for H 2 O 2 generation has been increasingly recognized in recent years, resulting in a number of focused studies to develop 2e‐ORR electrocatalysts . Nevertheless, the development of 2e‐ORR electrocatalysts has just begun, while the studies of 2D electrocatalysts for the 2e‐ORR are at the embryonic stage.…”

Section: D 2e‐orr Electrocatalystsmentioning

confidence: 99%

2D Electrocatalysts for Converting Earth‐Abundant Simple Molecules into Value‐Added Commodity Chemicals: Recent Progress and Perspectives

et al. 2019

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those emerging electrocatalytic redox reactions involving water, oxygen, and carbon dioxide as reactants. [7][8][9] The excellent progress achieved over the past decade has placed 2D electrocatalysts as one of the most important classes of nanostructured electrocatalysts. More significantly, 2D nanostructures are particularly useful for developing nonprecious-material-based electrocatalysts. For example, transition metal (TM) dichalcogenide (TMD)-based 2D nanomaterials have been used for water reduction to generate hydrogen via the hydrogen evolution reaction (HER). [10] In addition, 2D layered metal hydroxides (LMHs), [8d,11] layered metal oxides (LMO), [12] and 2D metal-organic frameworks (MOFs) [9c] have been developed for water oxidation to produce oxygen via the oxygen evolution reaction (OER). Graphene-based electrocatalysts have been used to achieve the 4-electron oxygen reduction reaction (ORR) [13] for fuel cells and the 2-electron oxygen reduction reaction (2e-ORR) [14] to produce hydrogen peroxide. Furthermore, ultrathin metal oxides [9b,15] or metal nanosheets, [16] TMDs, [9d,17] MXenes, [18] and 2D MOFs [19] have successfully been applied to convert nitrogen and carbon dioxide into ammonia and carbon fuels via the nitrogen reduction reaction (NRR) and carbon dioxide reduction reaction (CO 2 RR). The great success of nonprecious 2D electrocatalysts in a short time is due mainly to the unique 2D features that allow for the easy manipulation and engineering 2D nanostructures into catalytically active structures. As an emerging class of electrocatalysts, there are still several unexplored scientific domains and unrealized application potentials for 2D electrocatalysts. This aspect added to their unique 2D features and their advantages in creating catalytically active structures will continuously attract and motivate further research activities in the catalysis field. Meanwhile, a timely review on 2D electrocatalysts would undoubtedly facilitate this future research.The design, controllable synthesis, and applications of various types of 2D nanomaterials have been comprehensively covered by numerous excellent reviews. [2d,e,5] A number of excellent reviews on 2D electrocatalysts can also be found in the literature. [10a,20-23] However, these reviews focused on the development of 2D electrocatalysts for extensively reported energy-related applications such as the HER, OER, and ORR. In recent years, 2D electrocatalysts have increasingly been usedThe electrocatalytic conversion of earth-abundant simple molecules into value-added commodity chemicals can transform current chemical production regimes with enormous socioeconomic and environmental benefits. For these applications, 2D electrocatalysts have emerged as a new class of high-performance electrocatalyst with massive forward-looking potential. Recent advances in 2D electrocatalysts are reviewed for emerging applications that utilize naturally existing H 2 O, N 2 , O 2 , Cl − (seawater) and CH 4 (natural gas) as reactants for nitrogen reduction...

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“…Later, this method was modified by generating protons (H + ) through water oxidation which eliminated the direct purging of H 2 gas [9]. The major roadblock in this method is the development of a sustainable electrocatalyst for the selective reduction of oxygen to H 2 O 2 [19][20][21][22][23]. Today, most electrochemical H 2 O 2 production methods rely on precious-metal-based materials or transition metal and/or metal oxides, and hence their economic viability for the future technologies is highly questionable [10,[24][25][26][27].…”

Section: Introductionmentioning

confidence: 99%

Electrochemically derived functionalized graphene for bulk production of hydrogen peroxide

Yeddala¹,

Thakur²,

Anugraha³

et al. 2020

Beilstein J. Nanotechnol.

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On-site peroxide generation via electrochemical reduction is gaining tremendous attention due to its importance in many fields, including water treatment technologies. Oxidized graphitic carbon-based materials have been recently proposed as an alternative to metal-based catalysts in the electrochemical oxygen reduction reaction (ORR), and in this work we unravel the role of C=O groups in graphene towards sustainable peroxide formation. We demonstrate a versatile single-step electrochemical exfoliation of graphite to graphene with a controllable degree of oxygen functionalities and thickness, leading to the formation of large quantities of functionalized graphene with tunable rate parameters, such as the rate constant and exchange current density. Higher oxygen-containing exfoliated graphene is known to undergo a two-electron reduction path in ORR having an efficiency of about 80 ± 2% even at high overpotential. Bulk production of H 2 O 2 via electrolysis was also demonstrated at low potential (0.358 mV vs RHE), yielding ≈34 mg/L peroxide with highly functionalized (≈23 atom %) graphene and ≈16 g/L with low functionalized (≈13 atom %) graphene, which is on par with the peroxide production using state-of-the-art precious-metal-based catalysts. Hence this method opens a new scheme for the single-step large-scale production of functionalized carbon-based catalysts (yield ≈45% by weight) that have varying functionalities and can deliver peroxide via the electrochemical ORR process. 432

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Selective Electrochemical H₂O₂ Production through Two‐Electron Oxygen Electrochemistry

Cited by 555 publications

References 174 publications

Exploring Bi₂Te₃ Nanoplates as Versatile Catalysts for Electrochemical Reduction of Small Molecules

Exploring Bi₂Te₃ Nanoplates as Versatile Catalysts for Electrochemical Reduction of Small Molecules

2D Electrocatalysts for Converting Earth‐Abundant Simple Molecules into Value‐Added Commodity Chemicals: Recent Progress and Perspectives

Electrochemically derived functionalized graphene for bulk production of hydrogen peroxide

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Selective Electrochemical H2O2 Production through Two‐Electron Oxygen Electrochemistry

Cited by 555 publications

References 174 publications

Exploring Bi2Te3 Nanoplates as Versatile Catalysts for Electrochemical Reduction of Small Molecules

Exploring Bi2Te3 Nanoplates as Versatile Catalysts for Electrochemical Reduction of Small Molecules

2D Electrocatalysts for Converting Earth‐Abundant Simple Molecules into Value‐Added Commodity Chemicals: Recent Progress and Perspectives

Electrochemically derived functionalized graphene for bulk production of hydrogen peroxide

Contact Info

Product

Resources

About

Selective Electrochemical H₂O₂ Production through Two‐Electron Oxygen Electrochemistry

Exploring Bi₂Te₃ Nanoplates as Versatile Catalysts for Electrochemical Reduction of Small Molecules

Exploring Bi₂Te₃ Nanoplates as Versatile Catalysts for Electrochemical Reduction of Small Molecules