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
Frontiers of Chemical Science and Engineering
·
2021
·Vol. 16
·期 4
·498-510
·
IF 4.204
Bo Jinxiao,Li Mei,Zhu Xinli,Ge Qingfeng,Han Jinyu,Wang Hua
The electrochemical conversion of CO 2 -H 2 O into CO-H 2 using renewable energy is a promising technique for clean syngas production. Low-cost electrocatalysts to produce tunable syngas with a potential-independent CO/H 2 ratio are highly desired. Herein, a series of N -doped carbon nanotubes encapsulating binary alloy nanoparticles (M x Ni-NCNT, M= Fe, Co) were successfully fabricated through the co-pyrolysis of mela-mine and metal precursors. The M x Ni-NCNT samples exhibited bamboo-like nanotubular structures with a large specific surface area and high degree of graphitization. Their electrocatalytic performance for syngas production can be tuned by changing the alloy compositions and modifying the electronic structure of the carbon nanotube through the encapsulated metal nanoparticles. Consequently, syngas with a wide range of CO/H 2 ratios, from 0.5:1 to 3.4:1, can be produced on M x Ni-NCNT. More importantly, stable CO/H 2 ratios of 2:1 and 1.5:1, corresponding to the ratio to produce biofuels by syngas fermentation, could be realized on Co 1 Ni-NCNT and Co 2 Ni-NCNT, respectively, over a potential window of −0.8 to −1.2 V versus the reversible hydrogen electrode. Our work provides an approach to develop low-cost and potential-independent electrocatalysts to effectively produce syngas with an adjustable CO/H 2 ratio from electrochemical CO 2 reduction.
研究领域:
材料科学
·
电化学
·
可再生能源
·
催化
✓ 已验证
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）