Dunfeng Gao

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Verified

Dunfeng verified their affiliation via an institutional email.

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• PhD
• Professor (Full) at Dalian Institute of Chemical Physics

Renewable energy-driven electrocatalytic nitrate reduction reaction presents a low-carbon and sustainable route for ammonia synthesis under mild conditions. Yet, the practical application of this process is currently hindered by unsatisfactory electrocatalytic activity and long-term stability. Herein we achieve high-rate ammonia electrosynthesis us...

Producing valuable chemicals like ethylene via catalytic carbon monoxide conversion is an important nonpetroleum route. Here we demonstrate an electrochemical route for highly efficient synthesis of multicarbon (C2+) chemicals from CO. We achieve a C2+ partial current density as high as 4.35 ± 0.07 A cm⁻² at a low cell voltage of 2.78 ± 0.01 V over...

Electrochemically converting CO2 to valuable chemicals holds great promise for closing the anthropogenic carbon cycle. Owing to complex reaction pathways and shared rate‐determining steps, directing the selectivity of CO2/CO electrolysis to a specific multicarbon product is very challenging. We report here a strategy for highly selective production...

Tuning catalyst microenvironments by electrolytes and organic modifications is effective in improving CO2 electrolysis performance. An alternative way is to use mixed CO/CO2 feeds from incomplete industrial combustion of fossil fuels, but its effect on catalyst microenvironments has been poorly understood. Here we investigate CO/CO2 co-electrolysis...

The CO 2 electroreduction reaction (CO 2 RR) to fuels and feedstocks is an attractive route to close the anthropogenic carbon cycle and store renewable energy. The generation of more reduced chemicals, especially multicarbon oxygenate and hydrocarbon products (C 2+ ) with higher energy densities, is highly desirable for industrial applications. How...

Electrochemical carbon monoxide reduction reaction (CORR) to produce multicarbon (C2+) oxygenates using renewable electricity is a promising carbon utilization pathway. However, the performance of this process suffers from low C2+ oxygenates selectivity and insufficient current density. Here, we employed a Cu–Ag bimetallic strategy to enhance the s...

Electrochemical carbon monoxide reduction reaction (CORR) to produce multicarbon (C2+) oxygenates using renewable electricity is a promising carbon utilization pathway. However, the performance of this process suffers from low C2+ oxygenates selectivity and insufficient current density. Here, we employed a Cu‐Ag bimetallic strategy to enhance the s...

The conversion and utilization of carbon dioxide (CO2) is one of the central topics in the energy and environmental research community. The development of electrocatalytic CO2 reduction technology is expected to bring more economic and environmental benefits to the carbon-neutral policy. Although researchers have conducted extensive and in-depth st...

Electrochemical CO2 conversion to high‐value chemicals and fuels has been extensively investigated as a promising carbon‐neutrality technology. To date, most studies are generally performed with pure or highly concentrated CO2 feeds, however, the composition of industrial flue gases is very complex, with a low CO2 concentration and impurities like...

Ethylene oxide (EO) and ethylene glycol (EG) are two important commodity chemicals and are industrially produced from petroleum-derived ethylene via thermocatalytic processes. The overoxidation of ethylene and the implementation of high temperature and pressure lead to substantial CO2 emission. Renewable energy-driven electrocatalysis provides a lo...

The electrochemical synthesis of ethylene oxide (EO) using ethylene and water under ambient conditions presents a low‐carbon alternative to existing industrial production process. Yet, the electrocatalytic ethylene epoxidation route is currently hindered by largely insufficient activity, EO selectivity, and long‐term stability. Here we report a sin...

The electrochemical synthesis of ethylene oxide (EO) using ethylene and water under ambient conditions presents a low‐carbon alternative to existing industrial production process. Yet, the electrocatalytic ethylene epoxidation route is currently hindered by largely insufficient activity, EO selectivity, and long‐term stability. Here we report a sin...

Producing chemicals and fuels via direct electrolysis of dilute CO2 derived from industrial point sources can improve the economic feasibility of CO2 electrolysis technology, yet it suffers from many challenges owing to unfavorable mass transport, reaction thermodynamics, and kinetics. Here we report a molecular enhancement strategy for direct elec...

Electrochemically converting CO2 to valuable chemicals holds great promise for closing the anthropogenic carbon cycle. Owing to complex reaction pathways and shared rate‐determining steps, directing the selectivity of CO2/CO electrolysis to a specific multi‐carbon product is very challenging. We report here a strategy for highly selective productio...

CO2 electrolysis is an emerging and promising carbon neutrality technology, but currently suffers from challenging selectivity issues at industrially relevant reaction rates. Selectivity control in CO2 electrolysis relies on the molecular understanding and manipulation of multiple parallel reaction pathways that are equally governed by catalyticall...

Catalyst degradation and product selectivity changes are two of the key challenges in the electrochemical reduction of CO2 on copper electrodes. Yet, these aspects are often overlooked. Here, we combine in situ X-ray spectroscopy, in situ electron microscopy, and ex situ characterization techniques to follow the long-term evolution of the catalyst...

The electrolyte effect has been key to the electrochemical CO2 reduction reaction (CO2RR) and has received extensive attention in recent years. Here we combined atomic force microscopy, quasi-in situ X-ray photoelectron spectroscopy, and in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) to study the...

Advanced in situ X‐ray absorption spectroscopy characterization of electrochemically co‐electrodeposited bi‐element copper alloy electrodes shows that zinc yields the formation of a stable cationic Cu species during the electroreduction of CO2 at high cathodic polarization. In contrast, the formation/stabilization of cationic Cu species in copper o...

CO2 electrolysis is a promising route for achieving net‐zero emission through decarbonization. To realize CO2 electrolysis toward practical application, beyond catalyst structures, it is also critical to rationally manipulate catalyst microenvironments such as the water at the electrode/electrolyte interface. Here, the role of interfacial water in...

As an important fossil energy, natural gas has played an important role as a fuel for power and heat generation. With the development of renewable energies under the pressure of the climate change and environmental conservation, there is an urge to turn the fossil fuel era to fossil chemicals era to meet the ever increasing demanding for carbon-con...

CO2 electrolysis converting CO2 into valuable fuels and chemicals powered by renewable electricity shows great promise for practical applications. However, it suffers from low energy efficiency and carbon efficiency due...

As an emerging technology for achieving carbon neutrality, the electrocatalytic CO2 reduction reaction (CO2RR) converts CO2 and water to valuable fuels and chemicals with power supply from renewable energy. Currently, the practical application of the CO2RR suffers from insufficient electrocatalytic performance in terms of selectivity, reaction rate...

Supported metal (oxide) clusters, with both rich surface sites and high atom utilization efficiency, have shown improved activity and selectivity for many catalytic reactions over nanoparticle and single atom catalysts. Yet, the role of cluster catalysts has been rarely reported in CO2 electroreduction reaction (CO2RR), which is a promising route f...

Electrocatalytic CO2 reduction reaction (CO2RR) is an attractive way to simultaneously convert CO2 into value-added fuels and chemicals as well as to store intermittent electricity derived from renewable energy. However, this process involves multiple proton and electron transfer steps and is kinetically sluggish, thus leading to low conversion eff...

Catalytic conversion of CO 2 into chemicals and fuels is a viable method to reduce carbon emissions and achieve carbon neutrality. Through thermal catalysis, electrocatalysis, and photo(electro)catalysis, CO 2 can be converted into a wide range of valuable products, including CO, formic acid, methanol, methane, ethanol, acetic acid, propanol, light...

Sn-based catalysts have been investigated as efficient catalysts for CO2 electroreduction toward formate production. However, they still suffer from insufficient current densities and narrow potential windows at high formate Faradaic efficiency. Herein, we developed defect-rich SnO2 (e-SnO2) with surface-covered hydroxyls groups in situ derived fro...

Electrocatalysis is a process dealing with electrochemical reactions in the interconversion of chemical energy and electrical energy. Precise synthesis of catalytically active nanostructures is one of the key challenges that hinder the practical application of many important energy-related electrocatalytic reactions. Compared with conventional wet-...

The electrochemical CO 2 reduction reaction (CO 2 RR) over Cu‐based catalysts shows a great prospect with converting CO 2 into multicarbon (C 2+ ) fuels and chemicals. Herein, we introduce an A 2 M 2 O 7 structure into Cu‐based catalyst through a solid‐state reaction synthesis method. The Cu 2 P 2 O 7 catalyst is electrochemically reduced to metall...

An accurate understanding of reaction mechanisms is crucial for the rational design of highly efficient catalytic materials for electrochemical CO2 reduction reaction (CO2RR). In situ characterization methods are powerful to reveal structure-performance correlations of working catalysts under reaction conditions. Electrochemical in situ Raman spect...

The electrochemical CO2 reduction reaction (CO2RR) over Cu‐based catalysts shows great potential for converting CO2 into multicarbon (C2+) fuels and chemicals. Herein, we introduce an A2M2O7 structure into a Cu‐based catalyst through a solid‐state reaction synthesis method. The Cu2P2O7 catalyst is electrochemically reduced to metallic Cu with a sig...

Electrochemical CO2 reduction (ECR) is one of the promising CO2 recycling technologies sustaining the natural carbon cycle and offering more sustainable higher‐energy chemicals. Zn‐ and Pb‐based catalysts have improved formate selectivity, but they suffer from relatively low current activities considering the competitive CO selectivity on Zn. Here,...

Electrochemical CO2 reduction reaction (CO2RR) to multicarbon hydrocarbon and oxygenate (C2+) products with high energy density and wide availability is of great importance, as it provides a promising way to achieve the renewable energy storage and close the carbon cycle. Herein we design a Cu‐CuI composite catalyst with abundant Cu⁰/Cu⁺ interfaces...

The electrocatalytic CO2 reduction reaction (CO2RR) driven by renewable energy is an efficient approach to achieve the conversion and utilization of CO2. In this context, CO2RR has become an emerging research focus in the field of electrocatalysis over the past decade. While a large number of nanostructured catalysts have been developed to accelera...

The electrochemical CO2 reduction reaction (CO2RR) powered by renewable electricity is a promising route to close the carbon cycle, but it suffers from low product selectivity and high overpotential. Here we develop nitrogen and boron co‐doped hollow carbon spheres (NB‐CS) through the pyrolysis of a mixture comprising low‐molecular‐weight phenolic...

A Cu-CuI composite catalyst achieves a remarkable C2+ partial current density of 591 mA cm⁻² at −1.0 V vs. RHE, substantially higher than Cu or CuI alone. It is ascribed to the presence of residual Cu⁺ and adsorbed iodine species which improve CO adsorption and facilitate C−C coupling during CO2 electroreduction. Abstract Electrochemical CO2 reduc...

High‐voltage LiNi0.8Co0.1Mn0.1O2 (NCM811)‐based Li‐ion batteries (LIBs) with enhanced performance can be achieved by properly tailoring the electrolyte systems. Benzoic anhydride (BA) was proposed here as a promising bifunctional electrolyte additive that can not only construct a robust cathode‐electrolyte interface (CEI) film on the electrode surf...

Owing to unique electronic structure and high atom utilization, single-atom catalysts (SACs) have displayed unprecedented activity and selectivity toward a wide range of catalytic reactions, including electrocatalytic CO2 reduction reaction (CO2RR), which holds great promise in reducing carbon emission and storing renewable energy. The activity and...

Developing copper‐free catalysts for CO2 conversion into hydrocarbons and oxygenates is highly desirable for electrochemical CO2 reduction reaction (CO2RR). Herein, we report a cobalt phthalocyanine (CoPc) and zinc–nitrogen–carbon (Zn‐N‐C) tandem catalyst for CO2RR to CH4. This tandem catalyst shows a more than 100 times enhancement of the CH4/CO p...

Electrocatalytic CO2 reduction to liquid fuels and chemical feedstock, powered by renewable electricity, is an important approach for storing renewable energy and closing carbon cycle. Here, we study the pH effect on CO2 electroreduction selectivity over size-selected Au nanoparticles (NPs) in citrate buffer solutions with pH 3.7–6.0. A maximum CO...

Revealing the active nature of oxide derived copper (OD-Cu) is of key importance to understand its remarkable catalytic performance during the cathodic CO2 reduction reaction (CO2RR) to produce valuable hydrocarbons. Using advanced spectroscopy, electron microscopy and electro active surface area characterization techniques, the electronic structur...

Copper-indium bimetallic catalysts with a dendritic structure are fabricated by a two-step electrodeposition method using a hydrogen evolution template for the CO2 electroreduction reaction (CO2RR). The dendritic Cu-In-30 catalyst electrodeposited for 30 min shows the highest specific surface area and exposes the most active sites, resulting in imp...

CO2 is first electrochemically reduced into CO over CoPc. The CO then diffuses onto Zn‐N‐C for further conversion into CH4 over the Zn‐N4 site, decoupling the CO2 electroreduction pathway on a single active site into a two‐step tandem reaction which shows a more than 100 times enhancement of the CH4/CO production rate ratio compared with CoPc or Zn...

Significant progress on electrocatalytic CO2 reduction reaction (CO2RR) has been achieved in recent years. However, the research and development of electrolyzer device for CO2RR is scarce. Here we use anion exchange membrane to develop zero-gap electrolyzers for CO2RR. The electrochemical properties of the electrolyzers with Pd/C and Cu cathodes ar...

The variation in the morphology and electronic structure of copper during the electroreduction of CO2 into valuable hydrocarbons and alcohols was revealed by combining in situ surface and bulk sensitive X-ray spectroscopies with electrochemical electron scanning microscopy. These experiments proved that the electrified interface surface and near-su...

Rational designing microstructure of electrode materials has been regarded as an effective solution for boosting the electrochemical activity. To improve the electrochemical performance of NiCo2S4 for asymmetric supercapacitors (ASCs), a three-dimensional waxberry-like open hollow NiCo2S4 is designed and fabricated via self-assembly by a facile two...

To develop a high-performance positive electrode for asymmetric supercapacitor (ASC), a novel Ni3V2O8@carbon nanotubes (CNTs) composite with three-dimensionally (3D) flower-like structure is designed and prepared through an in-situ hydrothermal method. The particularly open architecture self-assembled by interlacement of Ni3V2O8 nano-petals with a...

The electrochemical CO2 reduction reaction (CO2RR) to give C1 (formate and CO) products is one of the most techno‐economically achievable strategies for alleviating CO2 emissions. Now, it is demonstrated that the SnOx shell in Sn2.7Cu catalyst with a hierarchical Sn‐Cu core can be reconstructed in situ under cathodic potentials of CO2RR. The result...

CO2 zu Ameisensäure: Eine in situ rekonstruierte Sn/SnOx-Grenzfläche ermöglicht die Ameisensäurebildung durch Optimieren der Bindung des Intermediats HCOO* und Förderung des Faradayschen Wirkungsgrads von C1-Produkten, indem die konkurrierende Wasserstoffentwicklung unterdrückt wird. Dies ergibt einen hohen Faradayschen Wirkungsgrad, eine hohe Stro...

Reversible exsolution and dissolution of metal nanoparticles in perovskite has been investigated as an efficient strategy to improve CO2 electrolysis performance. However, fundamental understanding with regard to the reversible exsolution and dissolution of metal nanoparticles in perovskite is still scarce. Herein, in situ exsolution and dissolutio...

Production of multicarbon products (C2+) from CO2 electroreduction reaction (CO2RR) is highly desirable for storing renewable energy and reducing carbon emission. The electrochemical synthesis of CO2RR catalysts that are highly selective for C2+ products via electrolyte‐driven nanostructuring is presented. Nanostructured Cu catalysts synthesized in...

Elektrolytgetriebene Nanostrukturierung wird für die Synthese von hochselektiven Cu‐Katalysatoren zur CO2‐Elektroreduktion zu C2+‐Produkten genutzt (80 % Faradayscher Wirkungsgrad). Abgesehen von einer erhöhten Rauigkeit infolge der Vorbehandlung begünstigen die Sauerstoffspezies unterhalb der Oberfläche, die Cu⁺‐Spezies und die adsorbierten Haloge...

Solid oxide electrolysis cell (SOEC) has attracted increasing attention as a promising device for electrochemical CO2 reduction reaction (CO2RR) due to its high efficiency and fast kinetics. Exploring active cathode catalysts for CO2RR is highly desirable for the research and development of SOEC. Herein, in situ exsolved FeNi3 nanoparticles on Sr2F...

Redox-active copper catalysts with accurately prepared oxidation states (Cu0, Cu+ and Cu2+) and high selectivity to C2 hydrocarbon formation, from electrocatalytic cathodic reduction of CO2, were fabricated and characterized. The electrochemically prepared copper-redox electro-cathodes yield higher activity for the production of hydrocarbons at low...

The utilization of fossil fuels (i.e., coal, petroleum, and natural gas) as the main energy source gives rise to serious environmental issues, including global warming caused by the continuously increasing level of atmospheric CO2. To deal with this challenge, fossil fuels are being partially replaced by renewable energy such as solar and wind. How...

Electrochemical CO2 reduction reaction (CO2RR) powered by renewable electricity has emerged as a promising approach to alleviate global warming and energy depletion simultaneously. Notably, efficient catalysts containing earth-abundant elements to achieve high CO2RR performance are in great demand for future applications. Herein, carbon-supported g...

CO2 electroreduction reaction (CO2RR) to chemicals and fuels is of both fundamental and practical significance since it would lead to a more efficient storage of renewable energy while closing the carbon cycle. Here we report enhanced activity and selectivity for CO2RR to multicarbon hydrocarbons and alcohols (~69 % Faradaic efficiency and −45.5 mA...

Metal-organic frameworks (MOFs), combining the favorable characteristics of heterogeneous and homogeneous catalysts, have been explored as a novel class of model catalytic materials for understanding electrochemical CO2 reduction reaction (CO2RR). MOFs exhibit high Faradaic efficiency of CO2RR, but suffer from limited current density of CO2RR (typi...

In situ and operando spectroscopic and microscopic methods were used to gain insight into the correlation between the structure, chemical state, and reactivity of size‐ and shape‐controlled ligand‐free Cu nanocubes (Cu‐cubes) during CO2 electroreduction (CO2RR). Dynamic changes in the morphology and composition of Cu‐cubes supported on carbon were...

In situ and operando spectroscopic and microscopic methods were used to gain insight into the correlation between the structure, chemical state, and reactivity of size‐ and shape‐controlled ligand‐free Cu nanocubes (Cu‐cubes) during CO2 electroreduction (CO2RR). Dynamic changes in the morphology and composition of Cu‐cubes supported on carbon were...

The electrochemical CO2 reduction reaction (CO2RR), with water as a hydrogen source, has been attracting great attention due to its promising applications for carbon recycle utilization and renewable electricity storage. In order to drive the process economically, highly efficient catalysts are urgently needed to overcome the constraints of high ov...

As a sustainable pathway for energy storage and to close the carbon cycle, CO2 electroreduction has recently gained significant interest. We report here the role of the electrolyte, in particular, of halide ions on CO2 electroreduction over plasma-oxidized polycrystalline Cu foils. It was observed that halide ions such as I− can induce significantl...

Active-phase engineering is regularly utilized to tune the selectivity of metal nanoparticles (NPs) in heterogeneous catalysis. However, the lack of understanding of the active phase in electrocatalysis has hampered the development of efficient catalysts for CO2 electroreduction. Herein, we report the systematic engineering of active phases of Pd N...

Electrochemical reduction of CO2 provides a sustainable solution to address the intermittent renewable electricity storage while recycling CO2 to produce fuels and chemicals. Highly efficient catalytic materials and reaction systems are required to drive this process economically. This Review highlights the new trends in advancing the electrochemic...

Correction for ‘Electrochemical promotion of catalysis over Pd nanoparticles for CO2 reduction’ by Fan Cai et al., Chem. Sci., 2017, DOI: 10.1039/c6sc04966d.

Electrochemical promotion of catalysis (EPOC) has been shown to accelerate the rate of many heterogeneous catalytic reactions; however, it has rarely been reported in low-temperature aqueous electrochemical reactions. Herein, we report a significant EPOC effect for the CO2 reduction to generate formate over Pd nanoparticles (NPs) in a 1 M KHCO3 aqu...

Nanoporous zinc oxide (ZnO) is prepared by a hydrothermal method followed by thermal decomposition for electrocatalytic reduction of CO2. In situ X-ray absorption spectroscopy results indicate that ZnO is reduced to Zn under the electrolysis conditions for catalyzing CO2 electroreduction. The reduced nanoporous ZnO exhibits obviously higher CO Fara...

Silicon carbide (SiC) was extracted using CCl4 and NH3 at 800 °C to form a SiC core with a derived nitrogen-doped carbon shell (SiC@N–C), which is explored as a supporting material for iron nanoparticles encapsulated in nitrogen-doped carbon (Fe@N–C) due to its excellent corrosion resistance. The carbon shell around SiC is essential to successfully...

Replacing platinum for catalyzing hydrogen evolution reaction (HER) in acidic medium remains great challenges. Herein, we prepared few-layered MoS2 by ball milling as an efficient catalyst for HER in acidic medium. The activity of as-prepared MoS2 had a strong dependence on the ball milling time. Furthermore, Ketjen Black EC 300J was added into the...

Adsorbed hydrogen participates in electrocatalytic reduction of CO2 and competitive hydrogen evolution reaction (HER) simultaneously, and its reaction pathway greatly affects the activity and selectivity of CO2 reduction. In this work, we investigate pH effect on electrocatalytic reduction of CO2 over Pd and Pt nanoparticles (NPs) with a similar si...

Size effect has been regularly utilized to tune the catalytic activity and selectivity of metal nanoparticle (NPs). Yet, there has been a lack of understanding on size effect in the electrocatalytic reduction of CO2, an important reaction coupling with intermittent renewable energy storage and carbon cycle utilization. We report here a prominent si...

The hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) are important electrocatalytic processes in water electrolyzers. Identifying efficient non-precious metal catalysts for HER and OER remains a great challenge for applications in different kinds of electrolyzers. Herein, we report that cobalt nanoparticles encapsulated in nitr...

Carbon dioxide transformation to fuels or chemicals provides an attractive approach for its utilization as feedstock and its emission reduction. Herein, we report a gas-phase electrocatalytic reduction of CO2 in an electrolytic cell, constructed using phosphoric acid-doped polybenzimidazole (PBI) membrane, which allowed operation at 170 °C. Pt/C an...