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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Desulfurization performance of chemical looping conversion using red mud as an oxygen carrier

Hongming Jiang,Shuchang Yan,Jingzhi Yan,Chengyang Li,Yan Lin,Zengli Zhao,Zhen Huang,Hongyu Huang,Haibin Li

Red mud (RM) is an alkaline waste residue produced in the aluminum industry, which has a huge output and is difficult to treat. However, it can be used as raw material for preparing oxygen carrier (OC) for rich in Fe, Na and Ca. In this paper, three types of RM were selected, and the desulfurization performance and mechanism of RM OCs under different reaction conditions were discussed. The results show that the desulfurization capacity of RM OCs mainly comes from Na/Ca elements, while Fe 2 O 3 has no desulfurization capacity above 750 °C. WSRM OCs have good desulfurization performance, and the desulfurization efficiency of WS900 can reach 86.28 % at 900 °C, although high temperature is not conducive to sulfur fixation by RM OCs. WSRM OC prepared at 800–900 °C has good desulfurization activity, while the OC prepared at 1000 °C or above will have a significant decline in desulfurization performance. The components in RM OCs with desulfurization activity mainly include Na 2 Ti 3 O 7 and Ca in the form of Ca 2 SiO 4 and CaTiO 3 , while NaAlSiO 4 , Na 6 Al 4 Si 4 O 17 and Ca 2 Al 2 SiO 7 almost have no sulfur fixation capacity. The redox performance of the three RM OCs under multi-cycle conditions is little affected by H 2 S atmosphere; and WSRM OCs rich in Na and Ca have the best redox performance.

CAS / MDL: 1305-78-8 1344-95-2
研究领域: 环境工程 · 化学工程 · 材料科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2025 · IF 8.3

Thermodynamics and experimental analysis of Ni-modified oxygen carriers with carbon resistance for chemical looping dry reforming of methane

Yuanhui Shen,Yunlian Liu,Ying Pan,Hongguang Jin

Chemical looping dry reforming of methane (CL-DRM) represents an innovative CO 2 utilization technology that enables efficient conversion of CH 4 and CO 2 while producing high-quality syngas. To investigate the carbon resistance of oxygen carriers, we present a comprehensive analysis of carbon deposition mechanisms in CL-DRM from both thermodynamic and experimental perspectives, establishing a quantitative correlation between carbon deposition and oxygen carrier characteristics. Experimental validation confirmed the thermodynamic predictions. Utilizing an exsolution strategy, we successfully synthesized nano-Ni-modified iron-based perovskite, which demonstrated exceptional reactivity and carbon resistance at 800 °C. This work provides both theoretical and practical guidance for the development of advanced oxygen carriers in CL-DRM systems.

研究领域: 能源工程 · 化学工程 · 材料科学 · 环境科学 · 催化
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Carbon Energy · 2025 · IF 24.2

Tailoring an Fe–Ov–Ce–Triggered Phase-Reversible Oxygen Carrier for Intensified Chemical Looping CO2 Splitting

Zhao Sun,Kun Lei,Louise R. Smith,Nicholas F. Dummer,Richard J. Lewis,Haifeng Qi,Kieran J. Aggett,Stuart H. Taylor,Zhiqiang Sun,Graham J. Hutchings

Advanced oxygen carrier plays a pivotal role in various chemical looping processes, such as CO 2 splitting. However, oxygen carriers have been restricted by deactivation and inferior oxygen transferability at low temperatures. Herein, we design an Fe–O v –Ce–triggered phase-reversible CeO 2− x ·Fe·CaO ↔ CeO 2 ·Ca 2 Fe 2 O 5 oxygen carrier with strong electron-donating ability, which activates CO 2 at low temperatures and promotes oxygen transformation. Results reveal that the maximum CO 2 conversion and CO yield obtained with 50 mol% CeO 2− x ·Fe·CaO are, respectively, 426% and 53.6 times higher than those of Fe·CaO at 700°C. This unique multiphase material also retains exceptional redox durability, with no obvious deactivation after 100 splitting cycles. The addition of Ce promotes the formation of the Fe–O v –Ce structure, which acts as an activator, triggers CO 2 splitting, and lowers the energy barrier of C═O dissociation. The metallic Fe plays a role in consuming O 2− lattice transformed from Fe–O v –Ce, whereas CaO acts as a structure promoter that enables phase-reversible Fe 0 ↔ Fe 3+ looping.

CAS / MDL: 10031-43-3
研究领域: 材料科学 · 化学工程
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Catalysts · 2018 ·Vol. 8 ·期 7 ·257 · IF 3.465

Hydrogen Production from Chemical Looping Reforming of Ethanol Using Ni/CeO2 Nanorod Oxygen Carrier

Lin Li,Bo Jiang,Dawei Tang,Zhouwei Zheng,Cong Zhao

Chemical looping reforming (CLR) technique is a prospective option for hydrogen production. Improving oxygen mobility and sintering resistance are still the main challenges of the development of high-performance oxygen carriers (OCs) in the CLR process. This paper explores the performance of Ni/CeO2nanorod (NR) as an OC in CLR of ethanol. Various characterization methods such as N2adsorption-desorption, X-ray diffraction (XRD), Raman spectra, transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), H2temperature-programmed reduction (TPR), and H2chemisorption were utilized to study the properties of fresh OCs. The characterization results show the Ni/CeO2-NR possesses high Ni dispersion, abundant oxygen vacancies, and strong metal-support interaction. The performance of prepared OCs was tested in a packed-bed reactor. H2selectivity of 80% was achieved by Ni/CeO2-NR in 10-cycle stability test. The small particle size and abundant oxygen vacancies contributed to the water gas shift reaction, improving the catalytic activity. The covered interfacial Ni atoms closely anchored on the underlying surface oxygen vacancies on the (111) facets of CeO2-NR, enhancing the anti-sintering capability. Moreover, the strong oxygen mobility of CeO2-NR also effectively eliminated surface coke on the Ni particle surface.Keywords:chemical looping reforming;hydrogen;oxygen carrier;CeO2;nanorod

研究领域: 能源科学 · 材料科学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2025 · IF 8.3

Experimental study on composite oxygen carrier NiFe2O4/Sr4Fe6O13 in chemical looping reforming coupled with thermochemical water splitting

Shuting Min,Chenxuanzi Wang,Mingxuan Zhong,Yibo Guo,Bo Xiao,Tingting Xu,Xun Wang

In this study, a series of composite oxygen carriers (OCs) of NiFe 2 O 4 /Sr 4 Fe 6 O 13 (xNiySr 4 ) was synthesized by solid-phase synthesis method. The performance evaluation for syngas and hydrogen production was investigated in chemical looping reforming coupled with thermochemical water splitting using ethanol as fuel. The presence of NiFe 2 O 4 enhanced the lattice oxygen activity and intensified the reduction of Sr 4 Fe 6 O 13 . The Ni–Fe alloy was produced in fuel reactor (FR) and then promoted water splitting in steam reactor (SR) for hydrogen production. The presence of Sr 4 Fe 6 O 13 regulated the reactivity of NiFe 2 O 4 , which prevented the ethanol complete oxidation in FR and enhanced the syngas production. Additionally, the introduction of Sr 4 Fe 6 O 13 decreased the content of NiFe 2 O 4 and suppressed carbon deposition, which resulted in a high purity of hydrogen in SR. Moreover, the existence of Sr 4 Fe 6 O 13 mitigated the sintering of NiFe 2 O 4 . The composite oxygen carrier of NiFe 2 O 4 /Sr 4 Fe 6 O 13 exhibited better cyclic stability than the single NiFe 2 O 4 and Sr 4 Fe 6 O 13 oxygen carrier. The 0.4NiFe 2 O 4 /0.6Sr 4 Fe 6 O 13 oxygen carrier, termed as 4Ni6Sr 4 , exhibited a good performance for syngas and hydrogen production performance at 800 °C. A high syngas purity of 74.36% was observed with a yield of 1.05 Nm³/kg ethanol in FR. The hydrogen yield and purity in SR were 6.51 mmol/g OC and 96.60%, respectively.

CAS / MDL: 1633-05-2
研究领域: 能源科学 · 材料科学
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JOURNAL OF APPLIED POLYMER SCIENCE · 2014 ·Vol. 131 ·期 12 · IF 1.64

Biodegradable polymersomes from four-arm PEG-b-PDLLA for encapsulating hemoglobin

Wenliang Li,Wenjing Zhang,Xiuyun Yang,Zhigang Xie,Xiabin Jing

A series of four-arm star block copolymers poly(ethylene glycol)-block-poly( d,l -lactide) (PEG-PDLLA) with different hydrophobic length were synthesized by ring-opening polymerization of lactide and characterized using 1 H NMR and gel permeation chromatography (GPC). These copolymers could self-assemble in aqueous solution to form the vesicle structure with controlled size and morphologies. Transmission electron microscopy (TEM) and DLS show the polymersomes are spherical with diameter of 70∼500 nm. The polymersomes made by direct hydration of copolymer thin films in water exhibit the controllable ability of encapsulating hemoglobin under mild condition. The hemoglobin content in the polymersomes could reach to 35 wt %. More importantly, the encapsulated hemoglobin keeps its own bioactivity and is capable of binding oxygen. This hemoglobin-encapsulated four-arm PEG-PLA polymersomes could have the potential to be applied as an artificial oxygen carrier for transfusion. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014 , 131 , 40433.

研究领域: 生物材料 · 医学工程
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FUEL · 2024 · IF 6.7

Enhancement of Fe/Ce oxygen carrier performance in chemical looping dry reforming of methane

Jinrui Zhang,Tianlong Yang,Qiong Rao,Zhongrui Gai,Peng Li,Yuanhui Shen,Mingkai Liu,Ying Pan,Hongguang Jin

Chemical looping dry reforming of methane (CL-DRM) is a promising technology for production of syngas and the utilization of greenhouse gases, which highly relies on efficient oxygen carrier (OC) to facilitate the energy and material transfer. In this work, Fe 2 O 3 /CeO 2 oxygen carriers in physical and crystalline contact modes were synthesized and used for CL-DRM. The Fe 2 O 3 /CeO 2 crystal interface significantly promoted the oxygen release of both Fe 2 O 3 and CeO 2 . The completely reduced iron elements dispersed uniformly into the CeO 2 support and formed pure CeFeO 3 in the oxidation step. CeFeO 3 showed enhanced methane conversion rate (81.3 %), CO selectivity (96.6 %) and lower temperature sensitivity. The time-resolved reaction performance of Fe-Ce oxygen carriers was investigated to understand the relationship between the oxygen vacancy concentration and reactivity of Fe-Ce oxygen carrier. With the increasing concentration of oxygen vacancies, the oxygen carrier exhibited elevated activity and enhanced selectivity. The redox range of CL-DRM was then tuned to enhance the reaction conversion and product purity. In the deep reduction range of oxygen carrier, the deposited carbon also served as the active redox intermediate for chemical looping and enhanced both the reaction conversion rate and the product purity to nearly 100 %. These findings showcased rational methods for design and utilization of iron-based oxygen carriers and expanded the potential for chemical looping applications.

研究领域: 化学工程 · 能源科学
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FUEL · 2024 · IF 6.7

Enhanced oxygen migration in tailored lanthanum-based perovskite for solar-driven dry reforming of methane

Qiongqiong Jiang,Yu Xin,Jiaxin Xing,Yali Cao,Fan Sun,Xueli Xing,Hui Hong,Chao Xu,Hongguang Jin

CO 2 and methane are the first and second most important greenhouse gases (GHGs). Solar thermal chemical looping dry reforming of methane (STCL-DRM) is a promising route to reduce methane/CO 2 emissions and achieve solar-to-chemical production. However, the lack of suitable oxygen carrier (OC) catalysts impedes the development. In this study, the tailored lanthanum-based perovskite by Cu and Ni substitution was synthesized as the OC catalyst. In the partial oxidation of methane, the tailored perovskite LaCu 0.5 Ni 0.5 O 3 can be reduced at the temperature of 450 °C–750 °C, and later the consumed lattice oxygen was supplemented through CO 2 reduction. Based on the DFT calculations, LaCu 0.5 Ni 0.5 O 3 exhibited a lower oxygen vacancy formation energy of 0.78 eV and a lower energy barrier of 0.32 eV for the oxygen migration from the second to the first layer. Compared to the undoped lanthanum-nickel perovskite and ceria, LaCu 0.5 Ni 0.5 O 3 shows superior oxygen migration ability. The enhanced oxygen migration and synergistic effect of Cu and Ni substitution were identified and unveiled through thermodynamic and computational study. The fixed-bed reactor tests yielded outstanding results with methane conversion >83 %, CO selectivity >97 %, and near-complete CO 2 conversion at 650 °C. Furthermore, we evaluated two pathways, STCL-DRM using LaCu 0.5 Ni 0.5 O 3 and traditional steam methane reforming (SMR), for methanol/acetic acid production. The proposed STCL-DRM process using LaCu 0.5 Ni 0.5 O 3 demonstrated ∼86 % reduction in energy demand compared to SMR while enabling negative CO 2 production. This process showed a carbon efficiency of roughly 81.9 %, which was 5 % higher than traditional SMR. These results show that the STCL-DRM can provide a competitive route for realizing solar thermochemical CO 2 reduction, clean conversion of methane, and efficient solar-to-chemical production.

研究领域: 材料科学 · 能源化学 · 环境科学
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ENERGY & FUELS · 2020 · IF 3.421

Chemical Looping Reforming of Glycerol for Continuous H2 Production by Moving-Bed Reactors: Simulation and Experiment

Bo Jiang,Lin Li,Qian Zhang,Jing Ma,Haotian Zhang,Jun Bai,Zhoufeng Bian,Binlin Dou,Sibudjing Kawi,Dawei Tang

Chemical looping reforming of biomass is a promising avenue for hydrogen generation. Both the design of reactor configurations and the screening of oxygen carriers represent major challenges in chemical looping technologies. Here, we synthesize three oxygen carriers (referred to as Ni–Al, NiW–Al, and W–Al) by a continuous coprecipitation method and first test them in a fixed-bed reactor. The NiW–Al showed the highest coke resistance, reducibility, and glycerol conversion. We employ an Ellingham diagram to explain the superior performance of the NiW–Al and screen operational temperatures from the standpoint of thermodynamics. Then, using the NiW–Al oxygen carriers, we investigate the effect of Ni-to-glycerol ratio, fuel reactor temperature, and steam-to-glycerol ratio in moving-bed reactors. Establishing two sets of five-stage equilibrium models in Aspen Plus, we compare the experimental results with simulations, discovering good agreement with each other. An isothermal and coke-free operational window was optimized at a fuel reactor temperature of 650 °C, a Ni-to-glycerol ratio of 0.9, and a steam-to-glycerol ratio of 4.5, achieving an average H2 yield of 1.5 mol-H2/mol-C. This work highlights the promise of combining moving-bed reactors with oxygen carriers with high oxygen storage capacity to utilize biomass by chemical looping reforming for continuous H2 generation.

研究领域: 能源工程 · 化学工程
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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Iron oxides with gadolinium-doped cerium oxides as active supports for chemical looping hydrogen production

Dewang Zeng,Fengwen Kang,Yu Qiu,Dongxu Cui,Min Li,Li Ma,Shuai Zhang,Rui Xiao

Supporting materials are often employed to enhance the stability of iron oxides oxygen carriers, but the reactivity is compromised for the dilution of the active phase. Here, we report several iron oxides supported by ionic conducting gadolinium-doped cerium oxides (GDC) for efficient chemical looping hydrogen production. The results show that GDC support can simultaneously improve redox stability and activity. Specifically, the produced Fe 2 O 3 /Gd 0.3 Ce 0.7 O 3−δ exhibits a high hydrogen production rate of ~0.71 mmol·g −1 ·min −1 and hydrogen yield of ~10 mmol·g −1 with negligible decay through 20 redox cycle. When using methane as the reducing agent, Fe 2 O 3 /Gd 0.3 Ce 0.7 O 3−δ shows high methane conversion of 75.67% and much lower carbon deposition than Fe 2 O 3 . The high performance is attributed to the improved oxide ion-conductivity through the oxygen carrier, which is further verified as the ability of the GDC support to accelerate the oxygen diffusion in the bulk. The explored support effects in this work can be extended to design oxygen carrier materials with both high activity and stability.

研究领域: 材料科学 · 能源化学 · 催化化学 · 无机化学 · 清洁能源技术
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2020 · IF 7.864

Tuning the Support Properties toward Higher CO2 Conversion during a Chemical Looping Scheme

Dewang Zeng,Yu Qiu,Li Ma,Min Li,Dongxu Cui,Shuai Zhang,Rui Xiao

The chemical looping process is promising for CO2 conversion because of the much higher CO2 conversion efficiency than the photocatalytic and electrocatalytic processes. Conventional oxygen carriers have to include a high content of inert support, typically Al2O3, to avoid sintering, thus leading to a trade-off between reactivity and stability. Here, we propose the use of ion-conductive GdxCe2–xO2−δ (GDC) to prepare the supported oxygen carriers. The resulting Fe2O3/GDC materials achieve both high reactivity and stability. Fe2O3/Gd0.3Ce1.7O2−δ shows high CO productivity (∼10.79 mmol·g–1) and CO production rate (∼0.77 mmol·g–1·min–1), which are twofold higher than that of Fe2O3/Al2O3. The performance remains stable even after 30 cycles. The mechanism study confirmed the rate-limiting role of the oxygen-ion conductivity, and the GDC support enhanced the oxygen-ion conductivity of oxygen carriers during the redox reactions, thus leading to improved CO2 splitting performance. A roughly linear relationship between the oxygen-ion conductivity and CO2 yield is also obtained and verified in our testing conditions. This relation can be used to predict and select oxygen carriers with high CO2 splitting performance.

研究领域: 材料科学 · 环境科学 · 化学工程
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Journal of Cleaner Production · 2024 · IF 9.7

Non-chemically valorizing the retired cathode of ternary lithium-ion battery to high-performance oxygen carrier for chemical looping combustion

Zhihao Zhou,Runnan Huang,Chao Huang,Guangze Nie,Zhenkun Sun,Lunbo Duan

The high contents of Ni, Co, and Mn in the retired cathode of ternary lithium-ion battery (rCTLIB) make it a promising raw precursor for preparing value-added reactive materials. However, most strategies for valorizing the rCTLIB highly depend on chemical leaching of Ni, Co, and Mn through complex procedures that involve the use of harsh liquids. Valorizing the rCTLIB through simple physical pathways is highly promising. Chemical looping combustion (CLC) is an innovative technology for producing energy from fossil fuels while inherently separating the resulting CO 2 into a nearly pure stream for subsequent permanent storage or utilization. In this study, high-performance oxygen carrier (OC) materials for the CLC of syngas have been successfully synthesized using a facile and scalable method that physically pelletizes the rCTLIB with Al 2 O 3 binder. Performance tests show that the H 2 and CO conversions in CLC of syngas exceed 90% for all prepared OCs. This performance is comparable to that of popularly employed OCs based on supported oxides. Moreover, the obtained OCs physically prepared from the rCTLIB demonstrate high stability with respect to reactivity and oxygen transport capacity, indicating a high potential for valorizing the rCTLIB into high-performance materials for applications involving CO 2 capture.

CAS / MDL: 1344-28-1
研究领域: 材料科学 · 能源技术 · 环境工程
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