Nature Communications
·
2024
·Vol. 15
·期 1
·1-13
·
IF 14.7
Niu Wenzhe,Feng Jie,Chen Junfeng,Deng Lei,Guo Wen,Li Huajing,Zhang Liqiang,Li Youyong,Zhang Bo
The synthesis of multi-carbon (C 2+ ) fuels via electrocatalytic reduction of CO, H 2 O using renewable electricity, represents a significant stride in sustainable energy storage and carbon recycling. The foremost challenge in this field is the production of extended-chain carbon compounds (C n , n ≥ 3), wherein elevated * CO coverage (θ co ) and its subsequent multiple-step coupling are both critical. Notwithstanding, there exists a “seesaw” dynamic between intensifying * CO adsorption to augment θ co and surmounting the C-C coupling barrier, which have not been simultaneously realized within a singular catalyst yet. Here, we introduce a facilely synthesized lattice-strain-stabilized nitrogen-doped Cu (LSN-Cu) with abundant defect sites and robust nitrogen integration. The low-coordination sites enhance θ co and concurrently, the compressive strain substantially fortifies nitrogen dopants on the catalyst surface, promoting C-C coupling activity. The n-propanol formation on the LSN-Cu electrode exhibits a 54% faradaic efficiency and a 29% half-cell energy efficiency. Moreover, within a membrane electrode assembly setup, a stable n-propanol electrosynthesis over 180 h at a total current density of 300 mA cm −2 is obtained.
研究领域:
能源化学
·
材料科学
·
催化反应
✓ 已验证
DOI
PubMed
高影响因子
FUEL
·
2024
·
IF 6.7
Lei Liu,Zijian Zhou,Xingqiang Zhang,Yue Zhou,Pengxin Zeng,Xingyu Liang,Xiaowei Liu,Minghou Xu
The application of Co-based recyclable zero-carbon fuels, utilizing oxygen both as a heat transfer fluid and reactant, has gained significant attention as a potential solution to address the intermittency challenges associated with zero-carbon renewable sources. However, the widespread adoption of these fuels faces obstacles, particularly when industrial waste heat deviates from the optimal operational temperature range of 900–1000 °C. Despite efforts to modify operation temperatures, the underlying reaction mechanism remains unclear. To elucidate the crucial factors influencing the recovery process of Co-based recyclable zero-carbon fuels, the density functional theory (DFT) method was employed to analyze the deoxygenation process of the spinel structure. This is essential as the recovery and combustion process involve the dissociation and reconstruction of crystal structures. In this study, the desorption steps of oxygen were studied separately. After the complete desorption of the first layer atoms from the slab surface, the second layer is exposed. To ensure structure stability, the surface undergoes reconstruction. The analysis revealed that the concentration of oxygen vacancy of the same type on the slab surface significantly impacts the energy barrier of deoxygenation, particularly in the initial two stages. This finding is further supported by examining the deoxygenation process in Co 2 MO 4 (M=Mn, Mg, Ni, and Cu) fuels, as reported in previous studies. Notably, the surface energy emerged as a key parameter for these Co-based spinel structure fuels. Modifying the surface energy, by lowering it, was identified to enhance the structural stability to increase the recovery temperature. Conversely, improving the surface energy will decrease the stability and lower the recovery temperature. Understanding and manipulating these factors, as proposed in this study, offer avenues for tailoring Co-based recyclable zero-carbon fuels for various industrial processes. This work serves as a crucial guide for further research and development in this field, potentially unlocking new possibilities to broaden the operation temperature range and enhance the performance of these fuels.
研究领域:
能源科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2017
·Vol. 33
·期 8
·1614-1620
·
IF 0.767
WANG Xiao-Qiang,LIU Jiang,XIE Yong-Min,CAI Wei-Zi,ZHANG Ya-Peng,ZHOU Qian,YU Fang-Yong,LIU Mei-Lin
A direct carbon solid oxide fuel cell (DC-SOFC) stack was prepared with 3 tubular cells electrically connected in series. To increase carbon storage in the stack, the anode was fabricated outside the tubular cells so that carbon fuel can be loaded at the exterior of the stack, which
is more spacious than the interior. The 3-cell-stack is operated directly with carbon as the fuel and oxygen in ambient air as the oxidant. With a total effective area of 10.2 cm2 and a 5% (w) Fe-loaded activated carbon fuel of 17 g, the stack reveals a peak power of 4.1
W at 800°C. The stack discharged at a constant current of 1.0 A for 19 h, giving a charge capacity of 19 A·h and an energy capacity of 31.6 W·h, which are much higher than those of a similar stack with anode on the inside and carbon loaded at the interior. The high capacity
of our DC-SOFC opens up potential applications in portable devices.
研究领域:
能源科学
·
材料科学
✓ 已验证
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2017
·
IF 4.798
Jia Liu,Jinshuo Qiao,Hong Yuan,Jie Feng,Chao Sui,Zhenhua Wang,Wang Sun,Kening Sun
Ni modified Ce 0.6 Mn 0.3 Fe 0.1 O 2 (Ni-CMF) material is evaluated as an anode material for hybrid direct carbon fuel cell (HDCFC). The Temperature Programmed Reaction (TPR) and GC test results show that the Ni additive significantly promotes the oxidation of carbon and consequently accelerates the formation rate of CO. Moreover, the Ni-CMF material is found to show a high electrical conductivity compared to pure CMF in HDCFC operating conditions. Taking advantage of the excellent catalytic activity and high conductivity, the electrolyte-supported HDCFC with Ni-CMF anode shows a high maximum power density of 580.7 mW cm −2 at 800 °C, when activated carbon is used as the fuel. Furthermore, the cell displays good stability under galvanostatic operation at current density of 50 mA cm −2 at 750 °C. These results indicate that the designed Ni-CMF composite material has the potential to be developed as an alternative anode for HDCFCs.
研究领域:
材料科学
·
能源工程
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Lijun Fan,Jun Wang,Linzhe Zhao,Nianjun Hou,Tian Gan,Xueli Yao,Ping Li,Yicheng Zhao,Yongdan Li
Activated carbons (AC) pretreated with HNO 3 and NaOH are investigated as the fuel of direct carbon fuel cells. HNO 3 and NaOH treatments both increase the oxygen content and decrease the graphitization degree of AC. The amount of hydroxyl groups on the surface of AC increases after the treatments with HNO 3 and NaOH, and then decreases during the subsequent heating process in an inert atmosphere . On the contrary, the carbonyl and quinone groups on the surface of the activated carbon remain stable during the heating process. The activated carbon treated with HNO 3 shows the highest reactivity towards oxidation and reverse Boudouard reactions due to its lowest graphitization degree and highest oxygen content. The single cell with a 380 μm-thick yttria stabilized zirconia layer as the electrolyte and the activated carbon treated with HNO 3 as the fuel exhibits the lowest polarization and the highest maximum power density of 128 mW cm −2 at 800 °C.
研究领域:
材料科学
·
能源工程
✓ 已验证
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2017
·
IF 6.395
Kening Sun,Jia Liu,Jie Feng,Hong Yuan,Minjie He,Chunming Xu,Zhenhua Wang,Wang Sun,Jinshuo Qiao
B-site substituted Sr 2 Fe 1.4 X 0.1 Mo 0.5 O 6-δ (SFXM, X = Bi, Al and Mg) are evaluated as anode materials for hybrid direct carbon fuel cells (HDCFCs). The structure, morphology, conductivity and catalytic activity of the as-prepared SFXM anode are systematically investigated. Under a reducing atmosphere, the exsolution of metallic Fe from the SFXM perovskite lattice are demonstrated by the XRD , SEM and TEM observations. Further element valence analysis on reduced SFXM suggests the X doping significantly alters the Fe 3+ /Fe 2+ and Mo 6+ /Mo 5+ ratio, and thus beneficial to the intrinsic conductivity of SFXM. All these advantages are responsible for the good electrochemical performances of SFXM anodes. Meanwhile, among these SFXM anodes, the conductivity, catalytic activity and electrochemical performance all obey the order of SFBM > SFAM > SFMM. The maximum power densities of the La 0.8 Sr 0.2 Ga 0.8 Mg 0.2 O 3 electrolyte supported single cell with SFBM as the anode reaches 399, 287 and 141 mW cm −2 at 800 °C, 750 °C and 700 °C, respectively. Such designed B-site substitution perovskites have great potential to be applied as HDCFC anode materials.
研究领域:
材料科学
·
能源工程
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Runze Wang,Guoqing Li,Yuyao Ma,Tengpeng Wang,Bin Chen,Tao Wei,Dehua Dong
Hybrid direct carbon fuel cells (HDCFCs) are promising to achieve high power density, good fuel-electrode contact, and high carbon-fuel conversion efficiency due to increased reaction sites and hybrid routines of carbon utilization. However, the performance of HDCFC is greatly restricted by mass transfer and detrimental carbon deposition . The so-called CO–CO 2 shuttle process, i. e., the coupling of the electrochemical reaction of CO to CO 2 and subsequent discharge of CO 2 towards the C fuel surface for gasification, is the key mass transfer process needed to be optimized. This study demonstrates a novel high-performance HDCFCs anode by integrating C-gasification tandem catalysis in dendritic channel anode support ( t -HDCFCs), which greatly enhances the CO–CO 2 shuttle and mitigates carbon deposition. As a result, the t -HDCFC delivers a comparable or even higher electrochemical performance than the other HDCFCs under the same operation conditions, such as a peak power density of 556 mW cm −2 at 750 °C.
研究领域:
能源科学
·
材料科学
·
电化学工程
✓ 已验证
产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Tingting Han,Lin Li,Jinjin Zhang,Fangyong Yu,Haibin Sun,Jaka Sunarso,Naitao Yang
Direct carbon solid oxide fuel cells (DC-SOFCs) can convert solid carbon directly to electricity via electrochemical oxidation and require less investment compared to other liquid or gas-fed fuel cells. Anode characteristic is one of the important factors in achieving efficient and stable operation of DC-SOFCs. In this work, we have successfully designed and developed 2D multi-physics field models for DC-SOFCs with finger-like nickel-based anode (Cell-A) and traditional nickel-based anode (Cell-B), respectively. Simulation results revealed that the cell performance was significantly enhanced with increases in the anode porosity and decreases in the distance of carbon fuel to porous anode. More importantly, the anode featuring a finger-like pore structure assumed a pivotal role in cell performance. Specifically, Cell-A exhibited higher electrochemical performance compared to Cell-B due to the lower resistance for gas transport and more abundant amount of three-phase boundaries for electrochemical reactions. Experimental results verified the simulation findings by making and operating these two DC-SOFCs. The fabricated Cell-A with finger-like anode delivered higher power output of 858 and 371 mW cm −2 at 850 °C when fueled with hydrogen and activated carbon, respectively, relative to Cell-B with traditional anode. The beneficial characteristic of finger-like anode was further demonstrated by the ability of Cell-A to retain stable operation for 14.1 h at 100 mA with the fuel utilization of 15.8% at 850 °C. This study provides important guidance for the design and improvement of DC-SOFCs, and promotes the sustainable utilization of carbon resources.
研究领域:
能源科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2014
·
IF 5.211
Yongmin Xie,Weizi Cai,Jie Xiao,Yubao Tang,Jiang Liu,Meilin Liu
Solid oxide fuel cells (SOFCs), with yttrium stabilized zirconia (YSZ) as electrolyte, composite of strontium-doped lanthanum manganate (LSM) and YSZ as cathode, and cermet of silver and gadolinium-doped ceria (GDC) as anode, are prepared and tested with 5wt% Fe-loaded activated carbon as fuel and ambient air as oxidant. It is found that electricity and CO gas can be cogenerated in the direct carbon SOFCs through the electrochemical oxidation of CO and the Boudouard reaction . The gas–electricity cogeneration performances are investigated by taking the operating time of the DC-SOFCs as a measure of rate decrease of the Boudouard reaction. Three single cells and a two-cell-stack are tested and characterized in terms of electrical power output , CO production rate, electrical conversion efficiency, and overall conversion efficiency. It turns out that a rapid rate of the Boudouard reaction is necessary for getting high electrical power and CO production. Taking the emitted CO as part of the power output, an overall efficiency of 76.5% for the single cell, and of 72.5% for the stack, is obtained.
研究领域:
能源科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Omega
·
2022
·
IF 4.132
Xiaofeng Li,Xiaohui Liu,Jiamao Hao,Lijun Li,Yanfang Gao,Yousong Gu,Zhenzhu Cao,Jinrong Liu
A strong metal–support interaction (SMSI) type catalyst has been synthesized and applied to a molten hydroxide direct carbon fuel cell (MHDCFC) to enhance the reaction activity of the anode carbon fuel through the interaction between the metal Ni and the support CeO2. Two catalysts have been prepared by a direct precipitation method (denoted NiO@CeO2) and a hydrothermal method (denoted NiO-CeO2), which are reduced by H2 to obtain Ni@CeO2 and Ni-CeO2, respectively. X-ray photoelectron spectroscopy (XPS), Raman, and temperature-programmed hydrogen reduction (H2-TPR) analysis results show that there are obvious oxygen vacancies and a Ni-O-Ce interface structure in NiO-CeO2 and Ni-CeO2, which is induced by the interaction between Ni and CeO2. The calculation results of current density and power density show that the performance of the MHDCFC is significantly improved in the presence of Ni-CeO2. The function fitting curves of the logarithm of the reaction rate constant (ln k) and the reciprocal of the temperature (1/T) show that the slope of the curve is decreased significantly after the addition of Ni-CeO2. In combination with density functional theory (DFT), the anode carbon reaction path is simulated in the MHDCFC, and the calculation results show that the reaction energy for the anodic carbon to generate carbon dioxide is decreased by 1.03 eV in the presence of Ni-CeO2.
研究领域:
材料科学
·
能源技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2022
·
IF 9.794
Xiao Yang,Minjian Ma,Chunming Xu,Rongzheng Ren,Jinshuo Qiao,Wang Sun,Kening Sun,Zhenhua Wang
Hybrid direct carbon fuel cells (HDCFCs) present its inherent and unparalleled advantages in converting chemical energy from organic waste, biomass, and coal directly into clean energy with high efficiency. However, the progress of HDCFC technology continues to be hampered by the sluggish anode reaction kinetics. Herein, an effective design strategy for HDCFC anode is proposed, a Cu-modified Sr 2 Fe 1.3 Cu 0.2 Mo 0.5 O 6-δ (SFCM) perovskite oxide is developed to meet the requirements of intermediate-temperature HDCFC anode. The Cu-doping SFCM anode demonstrates excellent redox structural stability and catalytic activity. In addition, the electrolyte-supported single cell with Cu-doping SFCM anode has improved the peak power density from 285.5 mW cm −2 to 489.3 mW cm −2 at 800 °C with activated carbon as the fuel. The significantly enhanced anode catalytic activity is primarily due to the improved interfacial activity and chemical adsorption of CO. Therefore, the present work shows an effective strategy for designing and developing novel high-performance HDCFCs anode materials .
研究领域:
能源材料
·
电化学
·
燃料电池
·
功能材料
·
催化化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2016
·
IF 3.205
Fangyong Yu,Yapeng Zhang,Liang Yu,Weizi Cai,Lili Yuan,Jiang Liu,Meilin Liu
Solid oxide fuel cells (SOFCs) with thin yttrium-stabilized-zirconia (YSZ) electrolyte supported on composite anode of nickel-iron bimetal and YSZ are prepared and operated directly on Fe-loaded activated carbon fuel, without any liquid medium or purging gas. The composition of the anode is represented as Ni 1- x Fe x O δ ( x = 0, 0.05, 0.1, 0.2, 0.3)-YSZ. Experiment result shows that such kind of all-solid-state direct carbon solid oxide fuel cells (DC-SOFCs) perform well at 800 °C, giving maximum output power densities in the range of 425–529 mW cm −2 . Similar to the case of a SOFC operated on hydrogen fuel , a small amount of Fe addition into the Ni-based anode can improve the performance of a DC-SOFC and the optimum composition is x = 0.1. A DC-SOFC with Ni 0.9 Fe 0.1 O δ -YSZ anode, loaded with 2.5 g Fe-loaded activated carbon fuel, is steadily operated at a constant current density of 0.1 A cm −2 for 15 h at 800 °C. The anodes and the DC-SOFCs are characterized through XRD , AC impedance spectroscopy , and SEM measurements. The superior performance of the Fe-added anode is analyzed accordingly.
研究领域:
能源材料科学
·
燃料电池技术
✓ 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）