scholarly journals Polymer-metal complexes as emerging catalysts for electrochemical reduction of carbon dioxide

2021 ◽  
Author(s):  
Daniele Sassone ◽  
Juqin Zeng ◽  
Marco Fontana ◽  
Adriano Sacco ◽  
M. Amin Farkhondehfal ◽  
...  
Keyword(s):  
Carbon Dioxide ◽  
Low Cost ◽  
Conductive Polymer ◽  
Reduction Reaction ◽  
Single Atom ◽  
Emeraldine Base ◽  
Hydrogen Electrode ◽  
Polymer Metal ◽  
Binder Free ◽  
Metal Doped

AbstractA class of metal-doped polyanilines (PANIs) was synthesized and investigated as electrocatalysts for the carbon dioxide reduction reaction (CO2RR). These materials show good affinity for the electrode substrate and allow to obtain stable binder-free electrodes, avoiding the utilization of expensive ionomer and additives. The emeraldine-base polyaniline (EB-PANI), in absence of metal dopant, shows negligible electrocatalytic activity and selectivity toward the CO2RR. Such behavior significantly improves once EB-PANI is doped with an appropriate cationic metal (Mn, Cu or Sn). In particular, the Sn-PANI outperforms other metal-doped samples, showing a good turnover frequency of 72.2 h−1 for the CO2RR at − 0.99 V vs the reversible hydrogen electrode and thus satisfactory activity of metal single atoms. Moreover, the Sn-PANI also displays impressive stability with a 100% retention of the CO2RR selectivity and an enhanced current density of 4.0 mA cm−2 in a 10-h test. PANI, a relatively low-cost substrate, demonstrates to be easily complexed with different metal cations and thus shows high tailorability. Complexing metal with conductive polymer represents an emerging strategy to realize active and stable metal single-atom catalysts, allowing efficient utilization of metals, especially the raw and precious ones. Graphic abstract

Self-assembled iron-containing mordenite monolith for carbon dioxide sieving

Science ◽  
2021 ◽  
Vol 373 (6552) ◽  
pp. 315-320
Author(s):  
Yu Zhou ◽  
Jianlin Zhang ◽  
Lei Wang ◽  
Xili Cui ◽  
Xiaoling Liu ◽  
...  
Keyword(s):  
Carbon Dioxide ◽  
Gas Adsorption ◽  
Separation Efficiency ◽  
Low Cost ◽  
One Pot ◽  
Free Process ◽  
Binder Free ◽  
Self Assembled ◽  
Cost Efficient ◽  
Breakthrough Experiments

The development of low-cost, efficient physisorbents is essential for gas adsorption and separation; however, the intrinsic tradeoff between capacity and selectivity, as well as the unavoidable shaping procedures of conventional powder sorbents, greatly limits their practical separation efficiency. Herein, an exceedingly stable iron-containing mordenite zeolite monolith with a pore system of precisely narrowed microchannels was self-assembled using a one-pot template- and binder-free process. Iron-containing mordenite monoliths that could be used directly for industrial application afforded record-high volumetric carbon dioxide uptakes (293 and 219 cubic centimeters of carbon dioxide per cubic centimeter of material at 273 and 298 K, respectively, at 1 bar pressure); excellent size-exclusive molecular sieving of carbon dioxide over argon, nitrogen, and methane; stable recyclability; and good moisture resistance capability. Column breakthrough experiments and process simulation further visualized the high separation efficiency.

scholarly journals High-Throughput Screening Single-Atom Alloy for Electroreduction of Dinitrogen to Ammonia

2021 ◽  
Author(s):  
Guokui Zheng ◽  
Ziqi Tian ◽  
Xingwang Zhang ◽  
Liang Chen ◽  
Xu Qian ◽  
...  
Keyword(s):  
High Throughput Screening ◽  
Density Functional ◽  
Ammonia Synthesis ◽  
Density Functional Theory Calculations ◽  
Reduction Reaction ◽  
Single Atom ◽  
Functional Theory ◽  
Metal Doped ◽  
Single Atom Alloy ◽  
Single Atom Alloys

<p></p><p>Exploring electrocatalyst with high activity, selectivity and stability is essential for development of applicable electrocatalytic ammonia synthesis technology. By performing density functional theory calculations, we systematically investigated a series of transition-metal doped Au-based single atom alloys (SAAs) as promising electrocatalysts for nitrogen reduction reaction (NRR). For Au-based electrocatalyst, the first hydrogenation step (*N<sub>2</sub>→*NNH) normally determines the limiting potential of the overall reaction process. Compared with pristine Au(111) surface, introducing single atom can significantly enhance the binding strength of N<sub>2</sub>, leading to decreased energy barrier of the key step, i.e., ΔG(*N<sub>2</sub>→*NNH). According to simulation results, three descriptors were proposed to describe ΔG(*N<sub>2</sub>→*NNH), including ΔG(*NNH), <i>d</i>-band center, and . Eight doped elements (Ti, V, Nb, Ru, Ta, Os, W, and Mo) were initially screened out with limiting potential ranging from -0.75V to -0.30 V. Particularly, Mo- and W-doped systems possess the best activity with limiting potentials of -0.30 V, respectively. Then the intrinsic relationship between structure and the potential performance was further analyzed by using machine-learning. The selectivity, feasibility, stability of these candidates were also evaluated, confirming that SAA containing Mo, Ru ,Ta, and W could be outstanding NRR electrocatalysts. This work not only broadens the understating of SAA application in electrocatalysis, but also devotes to the discovery of novel NRR electrocatalysts.</p><br><p></p>

Metal-Doped Two-Dimensional Borophene Nanosheets for the Carbon Dioxide Electrochemical Reduction Reaction

2020 ◽  
Vol 124 (44) ◽  
pp. 24156-24163
Author(s):  
Xuejian Xu ◽  
Xiuli Hou ◽  
Jiajie Lu ◽  
Peng Zhang ◽  
Beibei Xiao ◽  
...  
Keyword(s):  
Carbon Dioxide ◽  
Electrochemical Reduction ◽  
Reduction Reaction ◽  
Two Dimensional ◽  
Metal Doped

scholarly journals Co-Zn-MOFs Derived N-Doped Carbon Nanotubes with Crystalline Co Nanoparticles Embedded as Effective Oxygen Electrocatalysts

Nanomaterials ◽  
2021 ◽  
Vol 11 (2) ◽  
pp. 261
Author(s):  
Wendi Zhang ◽  
Xiaoming Liu ◽  
Man Gao ◽  
Hong Shang ◽  
Xuanhe Liu
Keyword(s):  
Carbon Nanotubes ◽  
Low Cost ◽  
Three Dimensional ◽  
Reduction Reaction ◽  
Hydrogen Electrode ◽  
New Strategy ◽  
Different Temperatures ◽  
Alkaline Electrolytes ◽  
Electron Migration ◽  
Co Nanoparticles

The oxygen reduction reaction (ORR) is a crucial step in fuel cells and metal-air batteries. It is necessary to expand the range of efficient non-precious ORR electrocatalysts on account of the low abundance and high cost of Pt/C catalysts. Herein, we synthesized crystalline cobalt-embedded N-doped carbon nanotubes (Co@CNTs-T) via facile carbonization of Co/Zn metal-organic frameworks (MOFs) with dicyandiamide at different temperatures (t = 600, 700, 800, 900 °C). Co@CNTs- 800 possessed excellent ORR activities in alkaline electrolytes with a half wave potential of 0.846 V vs. RHE (Reversible Hydrogen Electrode), which was comparable to Pt/C. This three-dimensional network, formed by Co@CNTs-T, facilitated electron migration and ion diffusion during the ORR process. The carbon shell surrounding the Co nanoparticles resulted in Co@CNTs-800 being stable as an electrocatalyst. This work provides a new strategy to design efficient and low-cost oxygen catalysts.

scholarly journals Nitrogen and Cobalt Co-Coped Carbon Materials Derived from Biomass Chitin as High-Performance Electrocatalyst for Aluminum-Air Batteries

Catalysts ◽  
2019 ◽  
Vol 9 (11) ◽  
pp. 954 ◽  
Author(s):  
Mi Wang ◽  
Jian Ma ◽  
Haoqi Yang ◽  
Guolong Lu ◽  
Shuchen Yang ◽  
...  
Keyword(s):  
Carbon Material ◽  
High Performance ◽  
Low Cost ◽  
Reduction Reaction ◽  
Discharge Voltage ◽  
Limiting Current ◽  
Alkaline Electrolyte ◽  
Hydrogen Electrode ◽  
Onset Potential ◽  
Practical Applications

Development of convenient, economic electrocatalysts for oxygen reduction reaction (ORR) in alkaline medium is of great significance to practical applications of aluminum-air batteries. Herein, a biomass chitin-derived carbon material with high ORR activities has been prepared and applied as electrocatalysts in Al-air batteries. The obtained cobalt, nitrogen co-doped carbon material (CoNC) exhibits the positive onset potential 0.86 V vs. RHE (reversible hydrogen electrode) and high-limiting current density 5.94 mA cm−2. Additionally, the durability of the CoNC material in alkaline electrolyte shows better stability when compared to the commercial Pt/C catalyst. Furthermore, the Al-air battery using CoNC as an air cathode catalyst provides the power density of 32.24 mW cm−2 and remains the constant discharge voltage of 1.17 V at 20 mA cm−2. This work not only provides a facile method to synthesize low-cost and efficient ORR electrocatalysts for Al-air batteries, but also paves a new way to explore and utilize high-valued biomass materials.

scholarly journals Recent advances in single atom catalysts for the electrochemical carbon dioxide reduction reaction

2021 ◽  
Author(s):  
Jincheng Zhang ◽  
Weizheng Cai ◽  
Fang Xin Hu ◽  
Hongbin Yang ◽  
Bin Liu
Keyword(s):  
Carbon Dioxide ◽  
Carbon Emission ◽  
Carbon Dioxide Reduction ◽  
Reduction Reaction ◽  
Single Atom ◽  
Recent Advances ◽  
Promising Solution

The electrochemical carbon dioxide reduction reaction (CO2RR) offers a promising solution to mitigate carbon emission and at the same time generate valuable carbonaceous chemicals/fuels.

The emerging applications of metal phosphides in carbon dioxide reduction reaction

2021 ◽  
Author(s):  
Sihao Wang ◽  
Gaofu Li ◽  
Lei Chen ◽  
Zhi Li ◽  
Zhuoyan Wu ◽  
...  
Keyword(s):  
Carbon Dioxide ◽  
Electrical Conductivity ◽  
High Efficiency ◽  
Catalytic Mechanism ◽  
Low Cost ◽  
Carbon Dioxide Reduction ◽  
Reduction Reaction ◽  
Future Research ◽  
Practical Applications ◽  
Metal Phosphides

The development of low-cost and high-efficiency catalysts is very important to promote carbon dioxide reduction reaction (CO2RR). Metal phosphides (MPs) are promising catalysts for CO2 reduction because of their excellent electrical conductivity, good stability, high activity and selectivity. In this review, we summarize the latest progress of MPs in CO2RR from chemocatalysis, electrocatalysis and photocatalysis, and discuss in detail their advantages and catalytic mechanism. In the end, we provide some potential challenges and inspiring outlooks to serve as guidance for future research and practical applications of MPs in catalytic CO2 reduction.

scholarly journals Bismuth-Based Free-Standing Electrodes for Ambient-Condition Ammonia Production in Neutral Media

2020 ◽  
Vol 12 (1) ◽  
Author(s):  
Ying Sun ◽  
Zizhao Deng ◽  
Xi-Ming Song ◽  
Hui Li ◽  
Zihang Huang ◽  
...  
Keyword(s):  
Low Cost ◽  
Catalytic Performance ◽  
Reduction Reaction ◽  
Ambient Conditions ◽  
Free Standing ◽  
Hydrogen Electrode ◽  
Faradaic Efficiency ◽  
Long Term Stability ◽  
High Efficient ◽  
Neutral Media

AbstractElectrocatalytic nitrogen reduction reaction is a carbon-free and energy-saving strategy for efficient synthesis of ammonia under ambient conditions. Here, we report the synthesis of nanosized Bi2O3 particles grown on functionalized exfoliated graphene (Bi2O3/FEG) via a facile electrochemical deposition method. The obtained free-standing Bi2O3/FEG achieves a high Faradaic efficiency of 11.2% and a large NH3 yield of 4.21 ± 0.14 $$ \upmu{\text{g}}_{{{\text{NH}}_{3} }} $$ μ g NH 3  h−1 cm−2 at − 0.5 V versus reversible hydrogen electrode in 0.1 M Na2SO4, better than that in the strong acidic and basic media. Benefiting from its strong interaction of Bi 6p band with the N 2p orbitals, binder-free characteristic, and facile electron transfer, Bi2O3/FEG achieves superior catalytic performance and excellent long-term stability as compared with most of the previous reported catalysts. This study is significant to design low-cost, high-efficient Bi-based electrocatalysts for electrochemical ammonia synthesis.

scholarly journals Computational Screening of Doped Graphene Electrodes for Alkaline CO2 Reduction

2021 ◽  
Vol 8 ◽  
Author(s):  
Anand M. Verma ◽  
Karoliina Honkala ◽  
Marko M. Melander
Keyword(s):  
Electron Transfer ◽  
Electrode Materials ◽  
Co2 Reduction ◽  
Reduction Reaction ◽  
Alkaline Media ◽  
Hydrogen Electrode ◽  
Computational Screening ◽  
Alkaline Conditions ◽  
Doped Graphene ◽  
Metal Doped

The electrocatalytic CO2 reduction reaction (CO2RR) is considered as one of the most promising approaches to synthesizing carbonaceous fuels and chemicals without utilizing fossil resources. However, current technologies are still in the early phase focusing primarily on identifying optimal electrode materials and reaction conditions. Doped graphene-based materials are among the best CO2RR electrocatalysts and in the present work we have performed a computational screening study to identify suitable graphene catalysts for CO2RR to CO under alkaline conditions. Several types of modified-graphene frameworks doped with metallic and non-metallic elements were considered. After establishing thermodynamically stable electrodes, the electrochemical CO2RR to CO is studied in the alkaline media. Both concerted proton-coupled electron transfer (PCET) and decoupled proton and electron transfer (ETPT) mechanisms were considered by developing and using a generalization of the computational hydrogen electrode approach. It is established that the CO2 electrosorption and associated charge transfer along the ETPT pathway are of utmost importance and significantly impact the electrochemical thermodynamics of CO2RR. Our study suggests an exceptional performance of metal-doped nitrogen-coordinated graphene electrodes, especially 3N-coordinated graphene electrodes.

scholarly journals Atomically dispersed Fe atoms anchored on S and N–codoped carbon for efficient electrochemical denitrification

2021 ◽  
Vol 118 (33) ◽  
pp. e2105628118
Author(s):  
Jiacheng Li ◽  
Miao Li ◽  
Ning An ◽  
Shuo Zhang ◽  
Qinan Song ◽  
...  
Keyword(s):  
Low Cost ◽  
Catalyst Activity ◽  
Nitrate Removal ◽  
Catalytic Performance ◽  
High Reactivity ◽  
Single Atom ◽  
Experimental Investigations ◽  
Active Centers ◽  
Hydrogen Electrode ◽  
Removal Capacity

Nitrate, a widespread contaminant in natural water, is a threat to ecological safety and human health. Although direct nitrate removal by electrochemical methods is efficient, the development of low-cost electrocatalysts with high reactivity remains challenging. Herein, bifunctional single-atom catalysts (SACs) were prepared with Cu or Fe active centers on an N-doped or S, N–codoped carbon basal plane for N2 or NH4+ production. The maximum nitrate removal capacity was 7,822 mg N ⋅ g−1 Fe, which was the highest among previous studies. A high ammonia Faradic efficiency (78.4%) was achieved at a low potential (−0.57 versus reversible hydrogen electrode), and the nitrogen selectivity was 100% on S-modified Fe SACs. Theoretical and experimental investigations of the S-doping charge-transfer effect revealed that strong metal–support interactions were beneficial for anchoring single atoms and enhancing cyclability. S-doping altered the coordination environment of single-atom centers and created numerous defects with higher conductivity, which played a key role in improving the catalyst activity. Moreover, interactions between defects and single-atom sites improved the catalytic performance. Thus, these findings offer an avenue for high active SAC design.

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