Enhanced CO2 electroreduction efficiency through secondary coordination effects on a pincer iridium catalyst

2015 ◽  
Vol 51 (27) ◽  
pp. 5947-5950 ◽  
Author(s):  
Steven T. Ahn ◽  
Elizabeth A. Bielinski ◽  
Elizabeth M. Lane ◽  
Yanqiao Chen ◽  
Wesley H. Bernskoetter ◽  
...  
Keyword(s):  
Electrocatalytic Reduction ◽  
Pincer Ligand ◽  
Faradaic Efficiency ◽  
Iridium Catalyst ◽  
Co2 Electroreduction ◽  
Low Overpotential

An iridium trihydride complex supported by a bifunctional pincer ligand promotes the electrocatalytic reduction of CO2 to formate in with excellent Faradaic efficiency and low overpotential.

Electrocatalytic Reduction of NO3– to Ultrapure Ammonia on {200} Facet Dominant Cu Nanodendrites with High Conversion Faradaic Efficiency

2021 ◽  
pp. 8121-8128
Author(s):  
Shivaraj B. Patil ◽  
Ting-Ran Liu ◽  
Hung-Lung Chou ◽  
Yu-Bin Huang ◽  
Chia-Che Chang ◽  
...  
Keyword(s):  
High Conversion ◽  
Electrocatalytic Reduction ◽  
Faradaic Efficiency

scholarly journals Double sulfur vacancies by lithium tuning enhance CO2 electroreduction to n-propanol

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Chen Peng ◽  
Gan Luo ◽  
Junbo Zhang ◽  
Menghuan Chen ◽  
Zhiqiang Wang ◽  
...  
Keyword(s):  
Anion Vacancy ◽  
High Energy ◽  
Hydrogen Electrode ◽  
Cycle Number ◽  
Faradaic Efficiency ◽  
Flow Cells ◽  
Forming Mechanism ◽  
Co2 Electroreduction ◽  
Tuning Strategy ◽  
Partial Current

AbstractElectrochemical CO2 reduction can produce valuable products with high energy densities but the process is plagued by poor selectivities and low yields. Propanol represents a challenging product to obtain due to the complicated C3 forming mechanism that requires both stabilization of *C2 intermediates and subsequent C1–C2 coupling. Herein, density function theory calculations revealed that double sulfur vacancies formed on hexagonal copper sulfide can feature as efficient electrocatalytic centers for stabilizing both CO* and OCCO* dimer, and further CO–OCCO coupling to form C3 species, which cannot be realized on CuS with single or no sulfur vacancies. The double sulfur vacancies were then experimentally synthesized by an electrochemical lithium tuning strategy, during which the density of sulfur vacancies was well-tuned by the charge/discharge cycle number. The double sulfur vacancy-rich CuS catalyst exhibited a Faradaic efficiency toward n-propanol of 15.4 ± 1% at −1.05 V versus reversible hydrogen electrode in H-cells, and a high partial current density of 9.9 mA cm−2 at −0.85 V in flow-cells, comparable to the best reported electrochemical CO2 reduction toward n-propanol. Our work suggests an attractive approach to create anion vacancy pairs as catalytic centers for multi-carbon-products.

scholarly journals Polymer-supported CuPd nanoalloy as a synergistic catalyst for electrocatalytic reduction of carbon dioxide to methane

2015 ◽  
Vol 112 (52) ◽  
pp. 15809-15814 ◽  
Author(s):  
Sheng Zhang ◽  
Peng Kang ◽  
Mohammed Bakir ◽  
Alexander M. Lapides ◽  
Christopher J. Dares ◽  
...  
Keyword(s):  
State Of The Art ◽  
Metal Nanoparticle ◽  
Local Concentration ◽  
Electrocatalytic Reduction ◽  
Catalytic Current ◽  
Faradaic Efficiency ◽  
Nanoparticle Catalysts ◽  
Ultrafine Metal ◽  
Current Densities ◽  
Energy Strategies

Developing sustainable energy strategies based on CO2 reduction is an increasingly important issue given the world’s continued reliance on hydrocarbon fuels and the rise in CO2 concentrations in the atmosphere. An important option is electrochemical or photoelectrochemical CO2 reduction to carbon fuels. We describe here an electrodeposition strategy for preparing highly dispersed, ultrafine metal nanoparticle catalysts on an electroactive polymeric film including nanoalloys of Cu and Pd. Compared with nanoCu catalysts, which are state-of-the-art catalysts for CO2 reduction to hydrocarbons, the bimetallic CuPd nanoalloy catalyst exhibits a greater than twofold enhancement in Faradaic efficiency for CO2 reduction to methane. The origin of the enhancement is suggested to arise from a synergistic reactivity interplay between Pd–H sites and Cu–CO sites during electrochemical CO2 reduction. The polymer substrate also appears to provide a basis for the local concentration of CO2 resulting in the enhancement of catalytic current densities by threefold. The procedure for preparation of the nanoalloy catalyst is straightforward and appears to be generally applicable to the preparation of catalytic electrodes for incorporation into electrolysis devices.

scholarly journals CuZnAl-Oxide Nanopyramidal Mesoporous Materials for the Electrocatalytic CO2 Reduction to Syngas: Tuning of H2/CO Ratio

Nanomaterials ◽  
2021 ◽  
Vol 11 (11) ◽  
pp. 3052
Author(s):  
Hilmar Guzmán ◽  
Daniela Roldán ◽  
Adriano Sacco ◽  
Micaela Castellino ◽  
Marco Fontana ◽  
...  
Keyword(s):  
Noble Metals ◽  
Co2 Reduction ◽  
Reduction Process ◽  
Mesoporous Structure ◽  
Catalytic Performance ◽  
H2 Production ◽  
Ambient Conditions ◽  
Transfer Resistance ◽  
Faradaic Efficiency ◽  
Co2 Electroreduction

Inspired by the knowledge of the thermocatalytic CO2 reduction process, novel nanocrystalline CuZnAl-oxide based catalysts with pyramidal mesoporous structures are here proposed for the CO2 electrochemical reduction under ambient conditions. The XPS analyses revealed that the co-presence of ZnO and Al2O3 into the Cu-based catalyst stabilize the CuO crystalline structure and introduce basic sites on the ternary as-synthesized catalyst. In contrast, the as-prepared CuZn- and Cu-based materials contain a higher amount of superficial Cu0 and Cu1+ species. The CuZnAl-catalyst exhibited enhanced catalytic performance for the CO and H2 production, reaching a Faradaic efficiency (FE) towards syngas of almost 95% at −0.89 V vs. RHE and a remarkable current density of up to 90 mA cm−2 for the CO2 reduction at −2.4 V vs. RHE. The physico-chemical characterizations confirmed that the pyramidal mesoporous structure of this material, which is constituted by a high pore volume and small CuO crystals, plays a fundamental role in its low diffusional mass-transfer resistance. The CO-productivity on the CuZnAl-catalyst increased at more negative applied potentials, leading to the production of syngas with a tunable H2/CO ratio (from 2 to 7), depending on the applied potential. These results pave the way to substitute state-of-the-art noble metals (e.g., Ag, Au) with this abundant and cost-effective catalyst to produce syngas. Moreover, the post-reaction analyses demonstrated the stabilization of Cu2O species, avoiding its complete reduction to Cu0 under the CO2 electroreduction conditions.

CO2 reduction to formic acid at low overpotential on BDD electrodes modified with nanostructured CeO2

2019 ◽  
Vol 7 (30) ◽  
pp. 17896-17905 ◽  
Author(s):  
Enrico Verlato ◽  
Simona Barison ◽  
Yasuaki Einaga ◽  
Stefano Fasolin ◽  
Marco Musiani ◽  
...  
Keyword(s):  
Formic Acid ◽  
Co2 Reduction ◽  
Faradaic Efficiency ◽  
Low Overpotential

Nanostructured CeO2/BDD electrodes produce formic acid with good faradaic efficiency at very low overpotential (>40% at η ≈ 40 mV).

scholarly journals Tracking structural evolution: operando regenerative CeOx/Bi interface structure for high-performance CO2 electroreduction

2020 ◽  
Author(s):  
Ruichao Pang ◽  
Pengfei Tian ◽  
Hongliang Jiang ◽  
Minghui Zhu ◽  
Xiaozhi Su ◽  
...  
Keyword(s):  
High Performance ◽  
Density Functional ◽  
Structural Evolution ◽  
Density Functional Theory Calculations ◽  
Active Phase ◽  
Interface Structure ◽  
Operating Conditions ◽  
Faradaic Efficiency ◽  
Co2 Electroreduction ◽  
Water Activation

Abstract Unveiling the structural evolution and working mechanism of catalysts under realistic operating conditions is crucial for the design of efficient electrocatalysts for CO2 electroreduction, yet remains highly challenging. Here, by virtue of operando structural measurements at multiscale levels, it is identified under CO2 electroreduction conditions that an as-prepared CeO2/BiOCl precatalyst gradually evolves into CeOx/Bi interface structure with enriched Ce3+ species, which serves as the real catalytically active phase. The derived CeOx/Bi interface structure compared to pure Bi counterpart delivers substantially enhanced performance with a formate Faradaic efficiency approaching 90% for 24 hours in a wide potential window. The formate Faradaic efficiency can be further increased by using isotope D2O instead of H2O. Density functional theory calculations suggest that the regenerative CeOx/Bi interfacial sites can not only promote water activation to increase local *H species for CO2 protonation appropriately, but also stabilize the key intermediate *OCHO in formate pathway.

Synthesis and Characterization of (Cu, S) Co-doped SnO2 for Electrocatalytic Reduction of CO2 to Formate at Low Overpotential

2018 ◽  
Vol 5 (9) ◽  
pp. 1330-1335 ◽  
Author(s):  
Xueyan Hu ◽  
Huimin Yang ◽  
Minmin Guo ◽  
Mengting Gao ◽  
Erhui Zhang ◽  
...  
Keyword(s):  
Synthesis And Characterization ◽  
Electrocatalytic Reduction ◽  
Low Overpotential ◽  
Reduction Of Co2 ◽  
Co Doped ◽  
Electrocatalytic Reduction Of Co2

scholarly journals A Universal Principle to Accurately Synthesize Atomically Dispersed Metal–N4 Sites for CO2 Electroreduction

2020 ◽  
Vol 12 (1) ◽  
Author(s):  
Wanzhen Zheng ◽  
Feng Chen ◽  
Qi Zeng ◽  
Zhongjian Li ◽  
Bin Yang ◽  
...  
Keyword(s):  
Metal Atom ◽  
Peak Power ◽  
Electric Energy ◽  
Energy Output ◽  
Central Metal ◽  
Faradaic Efficiency ◽  
Onset Potential ◽  
Co Conversion ◽  
Co2 Electroreduction ◽  
Specific Selectivity

AbstractAtomically dispersed metal–nitrogen sites-anchored carbon materials have been developed as effective catalysts for CO2 electroreduction (CO2ER), but they still suffer from the imprecisely control of type and coordination number of N atoms bonded with central metal. Herein, we develop a family of single metal atom bonded by N atoms anchored on carbons (SAs–M–N–C, M = Fe, Co, Ni, Cu) for CO2ER, which composed of accurate pyrrole-type M–N4 structures with isolated metal atom coordinated by four pyrrolic N atoms. Benefitting from atomically coordinated environment and specific selectivity of M–N4 centers, SAs–Ni–N–C exhibits superior CO2ER performance with onset potential of − 0.3 V, CO Faradaic efficiency (F.E.) of 98.5% at − 0.7 V, along with low Tafel slope of 115 mV dec−1 and superior stability of 50 h, exceeding all the previously reported M–N–C electrocatalysts for CO2-to-CO conversion. Experimental results manifest that the different intrinsic activities of M–N4 structures in SAs–M–N–C result in the corresponding sequence of Ni > Fe > Cu > Co for CO2ER performance. An integrated Zn–CO2 battery with Zn foil and SAs–Ni–N–C is constructed to simultaneously achieve CO2-to-CO conversion and electric energy output, which delivers a peak power density of 1.4 mW cm−2 and maximum CO F.E. of 93.3%.

Electrocatalytic reduction of CO2to CO with 100% faradaic efficiency by using pyrolyzed zeolitic imidazolate frameworks supported on carbon nanotube networks

2017 ◽  
Vol 5 (47) ◽  
pp. 24867-24873 ◽  
Author(s):  
Ying Guo ◽  
Huijuan Yang ◽  
Xin Zhou ◽  
Kunlong Liu ◽  
Chao Zhang ◽  
...  
Keyword(s):  
Carbon Nanotube ◽  
Electrochemical Reduction ◽  
Electrocatalytic Reduction ◽  
Zeolitic Imidazolate Frameworks ◽  
Faradaic Efficiency ◽  
Carbon Nanotube Networks

100% faradaic efficiency is achieved in electrochemical reduction of CO2to COviacoupling between ZIFs and CNTs.

CO2 Electroreduction at Low Overpotential on Oxide-Derived Cu/Carbons Fabricated from Metal Organic Framework

2017 ◽  
Vol 9 (6) ◽  
pp. 5302-5311 ◽  
Author(s):  
Kun Zhao ◽  
Yanming Liu ◽  
Xie Quan ◽  
Shuo Chen ◽  
Hongtao Yu
Keyword(s):  
Metal Organic Framework ◽  
Co2 Electroreduction ◽  
Metal Organic ◽  
Low Overpotential ◽  
Organic Framework
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