Discovery of main group single Sb–N4 active sites for CO2 electroreduction to formate with high efficiency

2020 ◽  
Vol 13 (9) ◽  
pp. 2856-2863 ◽  
Author(s):  
Zhuoli Jiang ◽  
Tao Wang ◽  
Jiajing Pei ◽  
Huishan Shang ◽  
Danni Zhou ◽  
...  
Keyword(s):  
Active Sites ◽  
High Efficiency ◽  
Main Group ◽  
Single Atom ◽  
Carbon Nanosheets ◽  
Co2 Electroreduction

We discover that an Sb single atom material consisting of Sb–N4 moieties anchored on N-doped carbon nanosheets can serve as a CO2RR catalyst to produce formate with high efficiency.

Double Boosting Single Atom Fe-N4 Sites for High Efficiency O2 and CO2 Electroreduction

Carbon ◽  
2021 ◽  
Author(s):  
Huijuan Yang ◽  
Xingpu Wang ◽  
ShengBao Wang ◽  
Pengyang Zhang ◽  
Chi Xiao ◽  
...  
Keyword(s):  
High Efficiency ◽  
Single Atom ◽  
Co2 Electroreduction

scholarly journals Atomically dispersed Fe3+ sites catalyze efficient CO2 electroreduction to CO

Science ◽  
2019 ◽  
Vol 364 (6445) ◽  
pp. 1091-1094 ◽  
Author(s):  
Jun Gu ◽  
Chia-Shuo Hsu ◽  
Lichen Bai ◽  
Hao Ming Chen ◽  
Xile Hu
Keyword(s):  
Active Sites ◽  
Carbon Support ◽  
Single Atom ◽  
Electronic Coupling ◽  
X Ray ◽  
Precious Metal Catalysts ◽  
Co2 Electroreduction ◽  
X Ray Absorption ◽  
Partial Current ◽  
Modest Activity

Currently, the most active electrocatalysts for the conversion of CO2 to CO are gold-based nanomaterials, whereas non–precious metal catalysts have shown low to modest activity. Here, we report a catalyst of dispersed single-atom iron sites that produces CO at an overpotential as low as 80 millivolts. Partial current density reaches 94 milliamperes per square centimeter at an overpotential of 340 millivolts. Operando x-ray absorption spectroscopy revealed the active sites to be discrete Fe3+ ions, coordinated to pyrrolic nitrogen (N) atoms of the N-doped carbon support, that maintain their +3 oxidation state during electrocatalysis, probably through electronic coupling to the conductive carbon support. Electrochemical data suggest that the Fe3+ sites derive their superior activity from faster CO2 adsorption and weaker CO absorption than that of conventional Fe2+ sites.

scholarly journals Double-Atom Catalysts Provide a Molecular Platform for Oxygen Evolution

2019 ◽  
Author(s):  
Lichen Bai ◽  
Chia-Shuo Hsu ◽  
Duncan Alexander ◽  
Hao Ming Chen ◽  
Xile Hu
Keyword(s):  
Oxygen Evolution ◽  
Active Sites ◽  
Supported Catalysts ◽  
Single Atom ◽  
Bond Forming ◽  
Co2 Electroreduction ◽  
Anode Reaction ◽  
X Ray Absorption ◽  
General Synthesis

The oxygen evolution reaction (OER) is an essential anode reaction for the generation of solar and electric fuels through water splitting or CO2 electroreduction. Mixed metal oxides containing Co, Fe, or Ni prove to be the most promising OER electrocatalysts in alkaline medium. However, the active sites and reaction mechanisms of these catalysts are difficult to study due to their heterogeneous nature. Here we describe a general synthesis of Co, Fe, and Ni-containing double-atom catalysts from their single-atom precursors via in-situ electrochemical transformation. Atomic-resolution microscopy and operando X-ray absorption spectroscopy (XAS) reveal molecule-like bimetallic active sites for these supported catalysts. Based on electrokinetic and XAS data, we propose a complete catalytic cycle for each catalyst. These mechanisms follow a similar O-O bond forming step and all exhibit bimetallic cooperation. However, the mechanisms diverge in the site and source of OH- for O-O bond formation as well as the order of proton and electron transfer. Our work demonstrates double-atom catalysts as an attractive platform for fundamental studies of heterogeneous OER electrocatalysts.

scholarly journals Electronic regulation of Ni single atom by confined Ni nanoparticles for fast and energy-efficient CO2 electroreduction

2021 ◽  
Author(s):  
Wenhao Ren ◽  
Xin Tan ◽  
Chen Jia ◽  
Anna Krammer ◽  
Qian Sun ◽  
...  
Keyword(s):  
Active Sites ◽  
Cell Voltage ◽  
Single Atom ◽  
Ni Nanoparticles ◽  
Precious Metal Catalysts ◽  
Co Conversion ◽  
Co2 Electroreduction ◽  
Enhanced Adsorption ◽  
Direct Solid ◽  
Nanoparticle Catalyst

Abstract Electrocatalytic CO2 to CO conversion is approaching the industrial benchmark. Currently, Au electrodes show the best performance, whereas non-precious metal catalysts exhibit inferior activity. Here we show a densely populated Ni single-atom on nanoparticle catalyst (NiSA/NP) via direct solid-sate pyrolysis, where Ni nanoparticles donate electrons to Ni(i)-N-C sites via carbon nanotubes network, achieves a high CO current of 352 mA cm− 2 at -0.55 V vs RHE in an alkaline flow cell. When coupled with a NiFe-based oxygen evolution anode into a zero-gap membrane electrolyser, it delivers an industrial-relevant CO current of 310 mA cm− 2 at a low cell voltage of -2.3 V, corresponding to an overall energy efficiency of 57%. The superior CO2 electroreduction performance is attributed to the enhanced adsorption of key intermediate COOH* on electron-rich Ni single atom, together with the dense active sites.

Boosting oxygen reduction catalysis with abundant copper single atom active sites

2018 ◽  
Vol 11 (8) ◽  
pp. 2263-2269 ◽  
Author(s):  
Feng Li ◽  
Gao-Feng Han ◽  
Hyuk-Jun Noh ◽  
Seok-Jin Kim ◽  
Yalin Lu ◽  
...  
Keyword(s):  
Oxygen Reduction ◽  
Active Sites ◽  
Single Atom ◽  
Carbon Nanosheets ◽  
Copper Doping ◽  
Nitrogenated Carbon

Single atomic copper doping in ultrathin nitrogenated carbon nanosheets over 20.9 wt% was achieved, greatly boosting the oxygen reduction catalysis.

Boosting CO2 electroreduction to CO with abundant nickel single atom active sites

2021 ◽  
Author(s):  
Wei-juan Wang ◽  
Changsheng Cao ◽  
Kaiwen Wang ◽  
Tianhua Zhou
Keyword(s):  
Active Sites ◽  
Single Atom ◽  
Ni Catalyst ◽  
Faradaic Efficiency ◽  
Co2 Electroreduction ◽  
Facile Route

A facile route for a single-atom Ni catalyst (Ni–SAs–NC) with dense Ni–N4 active sites is reported; the as-prepared Ni–SAs–N4C shows a 98% faradaic efficiency (FE) at −0.65 V for CO generation.

scholarly journals Double-Atom Catalysts Provide a Molecular Platform for Oxygen Evolution

2019 ◽  
Author(s):  
Lichen Bai ◽  
Chia-Shuo Hsu ◽  
Duncan Alexander ◽  
Hao Ming Chen ◽  
Xile Hu
Keyword(s):  
Oxygen Evolution ◽  
Active Sites ◽  
Supported Catalysts ◽  
Single Atom ◽  
Bond Forming ◽  
Co2 Electroreduction ◽  
Anode Reaction ◽  
X Ray Absorption ◽  
General Synthesis

The oxygen evolution reaction (OER) is an essential anode reaction for the generation of solar and electric fuels through water splitting or CO2 electroreduction. Mixed metal oxides containing Co, Fe, or Ni prove to be the most promising OER electrocatalysts in alkaline medium. However, the active sites and reaction mechanisms of these catalysts are difficult to study due to their heterogeneous nature. Here we describe a general synthesis of Co, Fe, and Ni-containing double-atom catalysts from their single-atom precursors via in-situ electrochemical transformation. Atomic-resolution microscopy and operando X-ray absorption spectroscopy (XAS) reveal molecule-like bimetallic active sites for these supported catalysts. Based on electrokinetic and XAS data, we propose a complete catalytic cycle for each catalyst. These mechanisms follow a similar O-O bond forming step and all exhibit bimetallic cooperation. However, the mechanisms diverge in the site and source of OH- for O-O bond formation as well as the order of proton and electron transfer. Our work demonstrates double-atom catalysts as an attractive platform for fundamental studies of heterogeneous OER electrocatalysts.

Efficient CO2 electroreduction over pyridinic-N active sites highly exposed on wrinkled porous carbon nanosheets

2018 ◽  
Vol 351 ◽  
pp. 613-621 ◽  
Author(s):  
Hongqiang Li ◽  
Nan Xiao ◽  
Mingyuan Hao ◽  
Xuedan Song ◽  
Yuwei Wang ◽  
...  
Keyword(s):  
Porous Carbon ◽  
Active Sites ◽  
Carbon Nanosheets ◽  
Co2 Electroreduction ◽  
Pyridinic N

scholarly journals Atomically dispersed Ni in cadmium-zinc sulfide quantum dots for high-performance visible-light photocatalytic hydrogen production

2020 ◽  
Vol 6 (33) ◽  
pp. eaaz8447 ◽  
Author(s):  
D. W. Su ◽  
J. Ran ◽  
Z. W. Zhuang ◽  
C. Chen ◽  
S. Z. Qiao ◽  
...  
Keyword(s):  
Quantum Dots ◽  
Zinc Sulfide ◽  
Active Sites ◽  
Heterogeneous Catalysts ◽  
Surface Engineering ◽  
High Efficiency ◽  
Single Atom ◽  
Intrinsic Activity ◽  
Cadmium Zinc Sulfide ◽  
Cadmium Zinc

Catalysts with a single atom site allow highly tuning of the activity, stability, and reactivity of heterogeneous catalysts. Therefore, atomistic understanding of the pertinent mechanism is essential to simultaneously boost the intrinsic activity, site density, electron transport, and stability. Here, we report that atomically dispersed nickel (Ni) in zincblende cadmium–zinc sulfide quantum dots (ZCS QDs) delivers an efficient and durable photocatalytic performance for water splitting under sunlight. The finely tuned Ni atoms dispersed in ZCS QDs exhibit an ultrahigh photocatalytic H2 production activity of 18.87 mmol hour−1 g−1. It could be ascribed to the favorable surface engineering to achieve highly active sites of monovalent Ni(I) and the surface heterojunctions to reinforce the carrier separation owing to the suitable energy band structures, built-in electric field, and optimized surface H2 adsorption thermodynamics. This work demonstrates a synergistic regulation of the physicochemical properties of QDs for high-efficiency photocatalytic H2 production.

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