Nano Research
·
2021
·Vol. 15
·期 1
·528-534
·
IF 8.897
Shen Chenqi,Wang Pengtang,Li Leigang,Huang Xiaoqing,Shao Qi
Syngas (CO + H 2 ) is the incredibly important feedstock for producing synthetic fuels and various value-added chemicals. CO 2 electrochemical reduction to syngas is an environmental-friendly and sustainable approach, but still challenging to produce tunable syngas with a wide ratio of CO/H 2 . Herein, by modulating the structure and phase, we have successfully obtained a series of copper-indium (Cu-In) catalysts, which are efficient for producing syngas with tunable CO/H 2 ratios. A series of CuIn bimetallic catalysts with different structures from hollow sphere to two-layer hollow sphere and different phases from CuO to Cu 2 O are developed. We find that the CO and H 2 are the only gaseous products, in which the CO/H 2 ratios can be readily tuned from 1.2 ± 0.1 to 9.0 ± 1.5 by simply controlling the thermal annealing temperature. It also exhibits high durability during a 10-h test. The unique performance is attributed to the modulated In enrichment on the Cu surfaces during the CO 2 reduction reaction, which causes the differences in binding energies for key reaction intermediates, thus resulting in the tunable composition of syngas. The present work emphasizes a simple yet efficient phase and structure modulating strategy for designing potential electrocatalysts for producing syngas with widely tunable CO/H 2 ratios.
研究领域:
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Jiale Wang,Qian Xiang,Wencong Zhang,Fenglei Shi,Fan Li,Peng Tao,Chengyi Song,Wen Shang,Tao Deng,Jianbo Wu
Electrochemical CO2 reduction (ECR) into syngas is a promising method to reduce CO2 in the atmosphere. However, balancing the activity of ECR and hydrogen evolution reaction (HER) and controlling the stable CO/H2 ratios in a large potential range for the industrial desired syngas are still challenging. Herein, a low-cost Ni-doped ZnO nanosheet array on a zinc foil is synthesized via a convenient hydrothermal method to produce a controllable ratio of CO/H2 into syngas. Because of the lower impedance and larger electrochemical area, Ni-doped ZnO has a more significant current density. Furthermore, by adjusting the Ni doping content in the ZnO nanosheet, the activity of ECR and HER could be controlled, and the ratio of CO/H2 can be tuned from 0.1 to 4.5 over a wide potential range (−1.2 to −1.8 V vs reversible hydrogen electrode, RHE), surpassing most of the reported work. Such a wide range and stable ratio of CO/H2 in a broad potential range makes it possible to convert CO2 into feedstock for many essential chemical products.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Nano Research
·
2020
·Vol. 13
·期 12
·3206-3211
·
IF 8.183
Zhang Meng,Hu Zheng,Gu Lin,Zhang Qinghua,Zhang Linghui,Song Qian,Zhou Wei,Hu Shi
A series of carbon-based binary single-atom catalysts of Fe and Ni coordinated by nitrogen are fabricated using a glucose-chelating method. Depending on the Ni/Fe content, they exhibit a wide-range of controllable CO/H 2 ratio from 0.14 to 10.86, which is meaningful to specific chemical processes. The durability of the catalyst is evaluated over an 8-hour period with no significant degradation of activity. The variation of the faradaic efficiency with Ni/Fe content is justified by density-functional-theory based calculation of the reaction barrier in both hydrogen evolution and CO 2 reduction reactions.
研究领域:
催化
·
电化学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Xinyao Zou,Chao Ma,Ang Li,Zhan Gao,Zulipiya Shadike,Kun Jiang,Junliang Zhang,Zhen Huang,Lei Zhu
Electrochemical conversion of CO2 to the syngas hybrid with the Fischer–Tropsch (FT) process is a promising way to produce synthetic fuels from renewable energy sources. The product distribution in liquid hydrocarbons produced by FT synthesis has strong dependence on the CO/H2 ratio of the syngas feedstock. Herein, we demonstrated the feasibility of tuning the CO/H2 ratio at a wide range by developing nanoparticle-assisted Ni–Co binary single-atom catalysts for electrocatalytic production of syngas. By controlling the elemental proportion of Ni–Co in the composite catalysts, electrochemical reduction of CO2 to syngas with a tunable CO/H2 ratio from 0.3 to 27.6 was achieved. For the binary catalysts with a Ni–Co ratio of 1:1, the CO/H2 ratio maintains at 1.3–1.5 in a broad potential range from −0.59 to −0.83 V versus reversible hydrogen electrode (RHE) and the total current density reaches ∼32.2 mA/cm2 at −1.0 V versus RHE. The promotion effect of nanoparticles on Ni–Co single-atom catalysts was validated by partial removal of nanoparticles and further density functional theory (DFT) calculations. As revealed by DFT calculations, nanoparticles incorporated in single-atom sites take essential roles in facilitating the adsorption of CO2 and the formation of *COOH. The origin of CO2RR and hydrogen evolution reaction reactivities can be identified as Ni–N4 and Co–N4 single-atom sites, respectively. The dual active sites allow the facile control of the CO/H2 ratio of electrochemical converted syngas, and it will be beneficial to downstream production of diverse chemicals.
研究领域:
催化
·
电化学
·
材料科学
·
能源转换
·
可持续化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）