JOURNAL OF SOLID STATE ELECTROCHEMISTRY
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2023
·Vol. 27
·期 5
·1261-1268
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IF 2.5
Deng Hao-chen (Preston),Hao Qingzhu,Wang Yuhang
The COVID-19 pandemic that is still prevalent around the globe each day consumes massive disposable face masks and consequently lays a heavy burden on waste management. Meanwhile, the incineration of these medical wastes further escalates the already overwhelming carbon emission that leads to global warming and climate change. To offer a potential solution addressing medical waste and CO 2 emission challenges, we herein develop a synthetic protocol to upgrade face masks into Ni, N-doped graphene (Ni–N-C) sheet catalysts for selectively reducing CO 2 into CO electrochemically. The high specific surface area and the uniform dispersion of Ni active sites of the catalyst derived from a regular disposable face mask enable a near-unity CO Faradaic efficiency (FE) at the current density of 200 mA cm −2 . This study offers outside-of-the-box thinking to address environmental issues by turning medical wastes into CO 2 reduction catalysts.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
·
IF 14.7
Xue Jing,Dong Xue,Liu Chunxiao,Li Jiawei,Dai Yizhou,Xue Weiqing,Luo Laihao,Ji Yuan,Zhang Xiao,Li Xu,Jiang Qiu,Zheng Tingting,Xiao Jianping,Xia Chuan
Using renewable electricity to convert CO 2 into CO offers a sustainable route to produce a versatile intermediate to synthesize various chemicals and fuels. For economic CO 2 -to-CO conversion at scale, however, there exists a trade-off between selectivity and activity, necessitating the delicate design of efficient catalysts to hit the sweet spot. We demonstrate here that copper co-alloyed with isolated antimony and palladium atoms can efficiently activate and convert CO 2 molecules into CO. This trimetallic single-atom alloy catalyst (Cu 92 Sb 5 Pd 3 ) achieves an outstanding CO selectivity of 100% (±1.5%) at −402 mA cm −2 and a high activity up to −1 A cm −2 in a neutral electrolyte, surpassing numerous state-of-the-art noble metal catalysts. Moreover, it exhibits long-term stability over 528 h at −100 mA cm −2 with an FE CO above 95%. Operando spectroscopy and theoretical simulation provide explicit evidence for the charge redistribution between Sb/Pd additions and Cu base, demonstrating that Sb and Pd single atoms synergistically shift the electronic structure of Cu for CO production and suppress hydrogen evolution. Additionally, the collaborative interactions enhance the overall stability of the catalyst. These results showcase that Sb/Pd-doped Cu can steadily carry out efficient CO 2 electrolysis under mild conditions, challenging the monopoly of noble metals in large-scale CO 2 -to-CO conversion.
研究领域:
材料科学
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化学工程
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电化学
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可持续能源
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DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Da Wang,Ying Zhu,Weiting Yu,Zhiqiao He,Feilong Dong,Yi Shen,Tao Zeng,Xiaohui Lu,Jun Ma,Lizhang Wang,Shuang Song
Ag-based electrodes have emerged as important candidates for the industrial electrochemical CO 2 reduction reaction (eCO 2 RR) to form CO. Herein, an intrinsic versatile Ag electrode has been derived in situ from Ag-MOF on Ag foam (denoted as ER-AF), which exhibits the highest current density (57.2 mA cm −2 ) at a potential of −1.15 V vs. RHE reported to date for the formation of CO in a commonly used H-type cell. ER-AF has multiple-roles: The 3D dendrite structure promotes mass diffusion; the rich edges sites favor CO 2 adsorption and conversion, and the highly exposed (111) facet facilitates the desorption of CO. Their cooperating functions result in the remarkable performance of ER-AF in the eCO 2 RR to form CO. This work offers an effective strategy to achieve high eCO 2 RR activity and selectivity by assembling the active and stable sites together on the MOF-derived materials.
研究领域:
电化学
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材料科学
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催化
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DOI
高影响因子
ACS Applied Energy Materials
·
2018
·
IF 0
Bao-Xia Dong,She-Liang Qian,Fan-Yan Bu,Yi-Chen Wu,Li-Gang Feng,Yun-Lei Teng,Wen-Long Liu,Zong-Wei Li
Heterogeneous electrocatalysis provides better control of the chemical surroundings of the catalyst’s active site for improved performance, offers the possibility of overcoming drawbacks of deactivation caused by aggregation or dimerization in homogeneous condition, and permits the use of benign aqueous solutions. Employing metal–organic frameworks (MOFs) or covalent–organic frameworks (COFs) to support the active molecular catalyst of porphyrin for electrochemical conversion of CO2 to CO is a promising strategy. We have rationally introduced a 3D highly stable porphyrin-based MOF of PCN-222(Fe) into heterogeneous catalysis through the simple dip-coating method. The composite catalyst PCN-222(Fe)/C (mass ratio = 1:2) exhibited high catalytic performance for electrochemical conversion of CO2 to CO with 494 mV overpotential (where j = 1.2 mA cm–2) and maximum 91% FECO in a CO2-saturated 0.5 M KHCO3 aqueous solution, achieving a TOF of 0.336 site–1 s–1. The catalyst was found to retain its crystallinity and stability after 10 h of electrolysis at −0.60 V versus RHE (average FECO 80.4%; RHE, reversible hydrogen electrode), which generates 334 μmol of CO with the TOF of 0.012 s–1 (0.286 site–1 s–1). These results indicate that the PCN-222(Fe)/C has a substantial catalytic effect on the electrochemical reduction of CO2 due to the combination of the intrinsic activity of the porphyrin molecule, and the promising CO2 adsorption ability endowed by the conserved porosity, as well as the high conductivity of carbon black.
研究领域:
电化学
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催化
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材料科学
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环境化学
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DOI
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Jie Tian,Zhijian Wang,Yaqin Hou,Yatao Yang,Haijun Chen,Zhanggen Huang
Inorganic Bi-based halide perovskites have attracted significant attention in the field of CO 2 photoreduction due to their excellent optoelectronic conversion performance and low toxicity. However, the inherent strong localization of electron-hole pairs remains the main factors limiting charge carrier transport and CRR performance. In this work, CBSB-x NCs with different Bi/Sb ratios were synthesized assisted by ultrasound methods to manipulate carrier behavior and assess CRR performance. The photoelectrochemical properties revealed that incorporation of Sb effectively suppressed nonradiative recombination and improved transport efficiency of charge carriers. Among the bimetallic variants, CBSB-1 NCs exhibited enhanced catalytic performance in CO production, with a yield of 38.77 μmol·g −1 and a high selectivity of 96.53 %. In-situ DRIFTS and DFT calculations indicated that Sb as co-catalytic sites promote charge transfer at the Bi-Br-Sb interface, accelerate the rapid evolution of b-CO 3 2- to HCOO - and significantly reduce the reaction energy barrier of CO.
研究领域:
材料科学
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化学工程
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环境科学
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纳米技术
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光化学
✓ 已验证
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
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2018
·Vol. 24
·期 34
·8596-8602
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IF 5.16
Yong Xu,Jiang Mo,Zi-Cheng Fu,Su Liu,Zhi Yang,Wen-Fu Fu
Graphical A hybrid photocatalyst consisting of Co and Co 2 P nanoparticles embedded in N, P-codoped carbon nanosheets was used in a visible light-driven system for CO 2 -to-CO conversion. The catalytic system displayed a high CO production rate of up to 35 000 μmol h −1 g −1 with CO selectivity of 79.1 % in the first 3 h of reaction. Linear CO production at an exceptionally high rate of 63 000 μmol h −1 g −1 was observed in the first 1 h of photocatalytic reaction. Artificial photosynthesis has attracted wide attention, particularly the development of efficient solar light-driven methods to reduce CO 2 to form energy-rich carbon-based products. Because CO 2 reduction is an uphill process with a large energy barrier, suitable catalysts are necessary to achieve this transformation. In addition, CO 2 adsorption on a catalyst and proton transfer to CO 2 are two important factors for the conversion reaction, and catalysts with high surface area and more active sites are required to improve the efficiency of CO 2 reduction. Here, a visible light-driven system for CO 2 -to-CO conversion is reported, which consists of a heterogeneous hybrid catalyst of Co and Co 2 P nanoparticles embedded in carbon nanolayers codoped with N and P (Co-Co 2 P@NPC) and a homogeneous Ru II -based complex photosensitizer. The average generation rate of CO of the system was up to 35 000 μmol h −1 g −1 with selectivity of 79.1 % in 3 h. Linear CO production at an exceptionally high rate of 63 000 μmol h −1 g −1 was observed in the first hour of reaction. Inspired by this highly active catalyst, Co@NC and Co 2 P@NPC materials were also synthesized and their structure, morphology, and catalytic properties for CO 2 photoreduction were explored. The results showed that the nanoparticle size, partially adsorbed H 2 O molecules on the catalyst surface, and the hybrid nature of the systems influenced their photocatalytic CO 2 reduction performance.
研究领域:
材料科学
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催化
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光化学
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环境科学
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DOI
PubMed
高影响因子
CARBON
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2021
·
IF 9.594
Zhaozhao Zhu,Zhao Li,Xinxin Wei,Junjie Wang,Shuhao Xiao,Rong Li,Rui Wu,Jun Song Chen
Developing efficient and stable catalysts for electrochemical CO 2 reduction reaction (CO 2 RR) in a wide potential window is highly desirable for achieving carbon neutrality, but remains greatly challenging. Herein, we demonstrate a facile synthetic strategy to synthesize transition metal nickel-nitrogen-carbon (Ni-N-C) catalyst where nickel nanoparticles have been in-situ encapsulated into N-doped carbon nanotubes (Ni@NCNT) for CO 2 RR. Strikingly, the as-prepared Ni@NCNT catalyst shows a high CO Faradaic efficiency (>90%) in a wide potential range of −0.65 to −1.0 V versus reversible hydrogen electrode ( vs. RHE), a large current density of 16.3 mA cm −2 at −0.8 V vs . RHE and robust durability after a continuous electroreduction of 18 h. Density functional theory calculations suggest that compared to pure Ni (111) and Ni nanoparticles-free solid N-doped carbon nanorods (NCNR), Ni@NCNT can more effectively suppress H 2 evolution and stabilize ∗COOH intermediates without influencing ∗CO desorption, thus, giving rise to high activity and desirable selectivity toward CO 2 RR.
研究领域:
电化学
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材料科学
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催化
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环境科学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2022
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IF 10.383
An-An Zhang,Yu-Lin Li,Zhi-Bin Fang,Lei Xie,Rong Cao,Yangyang Liu,Tian-Fu Liu
Photocatalytic CO2 reduction is one of the most cost-effective and environmentally friendly techniques of converting CO2 into high-value compounds and/or fuels. However, the performance of most current photocatalytic CO2 reduction catalysts is less than satisfactory for practical applications. Here, we synthesized a heterogeneous structure by integrating Cu2O and a porphyrin hydrogen-bonded organic framework (PFC-45), which was then fabricated into a thin-film catalyst on carbolic paper (CP) using a facile electrophoretic deposition technology. With improved electron–hole separation efficiency and visible-light-harvesting ability, this film (PFC-45/Cu2O@CP) significantly enhanced CO2-to-CO photoreduction, exceeding 2.4 and 3.2 times that of PFC-45@CP and PFC-45/Cu2O particles, respectively. Remarkably, PFC-45/Cu2O@CP also exhibited high selectivity (99%) and outstanding activity (11.81 μmol g–1 h–1) for photocatalytic CO2 reduction in pure water without any sacrificial agent. This work demonstrates a new strategy to design photocatalysts for efficient CO2 reduction.
研究领域:
材料科学
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环境科学
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化学工程
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光化学
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产品关联
DOI
PubMed
高影响因子
ACS Catalysis
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2023
·
IF 12.9
Jialin Wang,Yu-Cheng Huang,Yiqing Wang,Hao Deng,Yuchuan Shi,Daixing Wei,Mingtao Li,Chung-Li Dong,Hui Jin,Samuel S. Mao,Shaohua Shen
A variety of atomically dispersed transition-metal-anchored nitrogen-doped carbon (M–N–C) electrocatalysts have shown encouraging electrochemical CO2 reduction reaction (CO2RR) performance, with the underlying fundamentals of central transition-metal atom determined CO2RR activity and selectivity yet remaining unclear. Herein, a universal impregnation-acid leaching method was exploited to synthesize various M–N–C (M: Fe, Co, Ni, and Cu) single-atom catalysts (SACs), which revealed d-orbital electronic configuration-dependent activity and selectivity toward CO2RR for CO production. Notably, Ni–N–C exhibits a very high CO Faradaic efficiency (FE) of 97% at −0.65 V versus RHE and above 90% CO selectivity in the potential range from −0.5 to −0.9 V versus RHE, much superior to other M–N–C (M: Fe, Co, and Cu). With the d-orbital electronic configurations of central metals in M–N–C SACs well elucidated by crystal-field theory, Dewar–Chatt–Duncanson (DCD) and differential charge density analysis reveal that the vacant outermost d-orbital of Ni2+ in a Ni–N–C SAC would benefit the electron transfer from the C atoms in CO2 molecules to the Ni atoms and thus effectively activate the surface-adsorbed CO2 molecules. However, the outermost d-orbital of Fe3+, Co2+, and Cu2+ occupied by unpaired electrons would weaken the electron-transfer process and then impede CO2 activation. In situ spectral investigations demonstrate that the generation of *COOH intermediates is favored over Ni–N–C SAC at relatively low applied potentials, supporting its high CO2-to-CO conversion performance. Gibbs free energy difference analysis in the rate-limiting step in CO2RR and hydrogen evolution reaction (HER) reveals that CO2RR is thermodynamically favored for Ni–N–C SAC, explaining its superior CO2RR performance as compared to other SACs. This work presents a facile and general strategy to effectively modulate the CO2-to-CO selectivity from the perspective of electronic configuration of central metals in M–N–C SACs.
研究领域:
材料科学
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电化学
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催化
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DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 10
·期 4
·1852-1860
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IF 12.732
Yuning Zhang,Hao Jiang,Dongfang Niu,Ingo Manke,Chao Yang,Minghui Zhu,Xinsheng Zhang,Renjie Chen
Nitrogen-doped carbon nanomaterials for electrochemical reduction of CO2 (CO2ER) to CO have been extensively investigated, evaluated, and applied recently. Nevertheless, their weak adsorption capacity for CO2 usually results in a rapidly decayed CO faradaic efficiency (FECO) in the course of pursuing a commercial CO current density (jCO) by increasing the overpotential. Herein, we axially graft pyridine molecules on nitrogen-doped carbon nanotubes to construct a metal-free composite electrocatalyst (Py-N4CNTs-800) with enhanced CO2 affinity for CO2ER to efficiently generate CO. Py-N4CNTs-800 exhibits a prominent FECO of 96% at −0.99 V (vs. reversible hydrogen electrode, RHE) with a desirable jCO of 18.4 mA cm−2, and FECO can even be maintained above 90% in a wide electrochemical potential window (−0.79 to −1.19 V). In situ infrared spectra unambiguously indicate that grafted axial pyridine molecules can facilitate the CO2 adsorption and suppress the occurrence of competitive hydrogen evolution reaction (HER). Density functional theory (DFT) calculations enlighten that the introduction of pyridine molecules could dramatically stabilize the key intermediate *COOH, which effectively accelerates the reaction kinetics rate. Notably, Py-N4CNTs-800 delivers a promising jCO of 217 mA cm−2 at −0.9 V in a flow cell, showing a bright prospect of function strengthened carbon nanomaterial for industrial applications.
研究领域:
材料科学
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电化学
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催化
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纳米技术
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DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2022
·Vol. 57
·期 1
·526-537
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IF 4.682
Xu Lin-Wei,Qian She-Liang,Dong Bao-Xia,Feng Li-Gang,Li Zong-Wei
Molecular complexes with active metal centers exhibit high activity and selectivity for electrochemical CO 2 reduction reaction (CO 2 RR), which represents a promising method for transforming greenhouse gas into valuable chemicals and feedstock. Using metal–organic frameworks (MOFs) to load the active molecular complexes then employing the combination with the carbonic conducting material may exhibit a beneficial effect for CO 2 RR. Herein, we obtained a composite catalyst named PCN-222(Fe)/CNTs, which was in situ synthesized through the solvothermal method that loads iron porphyrin-centered PCN-222(Fe) molecules onto CNTs. The catalyst PCN-222(Fe)/CNTs exhibits excellent electrocatalytic performance for CO 2 RR with a FE CO of 95.5% (m(Fe-TCPP):m(CNTs) = 1:30, written as PCN-222(Fe)/CNTs-30) and an overpotential ( η ) of 494 mV. In addition, the turnover frequency (TOF) is high as 448.76 h −1 (3.011 site −1 s −1 ) and the hydrogen evolution reaction (HER) is indistinctive. After long-term electrocatalysis of 10 h at −0.6 V vs. RHE, PCN-222(Fe)/CNTs-30 remained its high catalytic performance with average FE CO = 90%. This work provides a solid foundation for further research in the high-efficiency transformation of CO 2 to CO. Graphical abstract
研究领域:
电化学
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材料科学
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催化
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环境科学
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产品关联
DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-13
·
IF 16.6
Sun Ji Wei,Wu Xuefeng,Liu Peng Fei,Chen Jiacheng,Liu Yuanwei,Lou Zhen Xin,Zhao Jia Yue,Yuan Hai Yang,Chen Aiping,Wang Xue Lu,Zhu Minghui,Dai Sheng,Yang Hua Gui
Practical electrochemical CO 2 -to-CO conversion requires a non-precious catalyst to react at high selectivity and high rate. Atomically dispersed, coordinatively unsaturated metal-nitrogen sites have shown great performance in CO 2 electroreduction; however, their controllable and large-scale fabrication still remains a challenge. Herein, we report a general method to fabricate coordinatively unsaturated metal-nitrogen sites doped within carbon nanotubes, among which cobalt single-atom catalysts can mediate efficient CO 2 -to-CO formation in a membrane flow configuration, achieving a current density of 200 mA cm −2 with CO selectivity of 95.4% and high full-cell energy efficiency of 54.1%, outperforming most of CO 2 -to-CO conversion electrolyzers. By expanding the cell area to 100 cm 2 , this catalyst sustains a high-current electrolysis at 10 A with 86.8% CO selectivity and the single-pass conversion can reach 40.4% at a high CO 2 flow rate of 150 sccm. This fabrication method can be scaled up with negligible decay in CO 2 -to-CO activity. In situ spectroscopy and theoretical results reveal the crucial role of coordinatively unsaturated metal-nitrogen sites, which facilitate CO 2 adsorption and key *COOH intermediate formation.
研究领域:
材料科学
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电化学
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催化
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）