Materials Chemistry Frontiers
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2023
·Vol. 7
·期 16
·3382-3389
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IF 7
Gaoming Sun,Chong Zou,Wen Sun,Ying Fang,Shuijian He,Yana Liu,Jiguang Zhang,Yunfeng Zhu,Jun Wang
The electrochemical reduction of CO2 to value-added products represents a promising strategy to store renewable energy and realize global carbon neutrality. Bi-based materials have attracted extensive attention for formate production from CO2 reduction. Herein, we employ BiPbO2Br nanosheets as the bimetallic oxyhalide precursor to prepare a reconstructed Bi–Pb composite catalyst by electroreduction. The resultant catalyst exhibits impressive performance for formate production, including a high partial current density (40 mA cm−2 at −1.0 V), a high faradaic efficiency (96.6% at −0.9 V), a high energy conversion efficiency (>50% from −0.8 to −1.1 V), and good stability. As compared with the monometallic Bi and Pb counterparts, the Bi–Pb composite catalyst demonstrates superior intrinsic performance, which is attributed to the multiphase composites and abundant heterogeneous interfaces derived from electroreduction induced structural reconstruction of BiPbO2Br. This work offers an attractive strategy to further improve the performance of Bi catalysts for CO2 reduction to formate.
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ADVANCED MATERIALS
·
2023
·Vol. 35
·期 33
·2302325
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IF 29.4
Chang Guo,Fuli Zhang,Xiao Han,Lipeng Zhang,Qian Hou,Lele Gong,Jincheng Wang,Zhenhai Xia,Jianhua Hao,Keyu Xie
To date, the effect of noble metal (NM) electronic structures on CO 2 reaction activity remains unknown, and explicit screening criteria are still lacking for designing highly efficient catalysts in CO 2 -breathing batteries. Herein, by preferentially considering the decomposition of key intermediate Li 2 CO 3 , an intrinsic descriptor constituted of the d x 2 − y 2 ${{\rm{d}}}_{{x}^2 - {y}^2}$ orbital states and the electronegativity for predicting high-performance cathode material are discovered. As a demonstration, a series of graphene-supported noble metals (NM@G) as cathodes are fabricated via a fast laser scribing technique. Consistent with the preliminary prediction, Pd@G exhibits an ultralow overpotential (0.41 V), along with superior cycling performance up to 1400 h. Moreover, the overall thermodynamic reaction pathways on NM@G confirm the reliability of the established intrinsic descriptor. This basic finding of the relationship between the electronic properties of noble metal cathodes and the performance of Li-CO 2 batteries provides a novel avenue for designing remarkably efficient cathode materials for metal-CO 2 batteries.
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Journal of Physical Chemistry C
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2023
·
IF 3.7
Minglu Li,Siyu Kuang,Hai Liu,Qun Fan,Sheng Zhang,Xinbin Ma
Significant efforts have been devoted to the investigation of catalysts for converting CO2 into C2+ products. Cu catalysts are attractive for their initial selectivities but limited by the low stability over time. Herein we investigated the stability of Cu catalysts in an operating CO2RR environment. Hydroxides in electrolytes were found to play a key role in morphology evolution of Cu catalysts and thus result in decreasing Faradaic efficiencies of C2+ products. To this end, we deposited a porous carbon overlay on Cu catalysts through a thermal annealing method. Physical characterizations and electrochemical measurements showed that the morphology of Cu catalysts and Faradaic efficiencies of products were well maintained during the reaction. As evidenced by Fourier transform infrared spectroscopy with phenolphthalein as a probe, the added carbon overlay could effectively resist the influence of hydroxide corrosion on Cu catalysts. This study provides an efficient strategy to improve the stability of copper catalysts toward electrochemical CO2 reduction.
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Journal of CO2 Utilization
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2022
·
IF 8.321
Yuxiao Zhu,Wei Zhou,Zichao Dong,Xinxin Zhang,Zhipeng Chen,Ziyong Liu,Fuli Li,Jingxin Fan,Mingyang Jiao,Licheng Liu
Perovskite oxides have been widely used as catalyst due to their ordered structure, diverse chemical range and outstanding properties. However, there are few studies on the application of perovskite oxides in CO 2 electrocatalytic reduction reaction (CO 2 RR). In this paper, nanosized LaInO 3 perovskite catalyst was successfully synthesized and applied to CO 2 RR. It displays excellent activity for formate production. The highest faradaic efficiency of formate reaches 91.4 % and the partial current density of formate is 106.8 mA cm −2 at a moderate overpotential of 0.9 V. Additionally, in a wide potential range (−0.8 ∼ −1.3 V vs. RHE), the faradaic efficiency of formate is above 80 %, which is far better than In 2 O 3 (64.6 %) and the physical mixture of In 2 O 3 and La 2 O 3 (63.7 %). The experimental research and DFT calculations indicate that the outstanding activity of LaInO 3 is mainly owing to its intensive adsorption stability to free radical intermediates (CO 2 •─ ) and lower desorption free energy of formate products during reaction.
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Journal of Energy Chemistry
·
2022
·
IF 13.599
Huan Xie,Ruikuan Xie,Zhiyuan Zhang,Yongyu Pang,Yuting Luo,Jiong Li,Bilu Liu,Maria-Magdalena Titirici,Guoliang Chai
The conversion of CO 2 into value-added chemicals coupled with the storage of intermittent renewable electricity is attractive. CuO nanosheets with an average size and thickness of ∼ 30 and ∼ 20 nm have been developed, which are in situ reduced into Cu nanosheets during electrochemical CO 2 reduction reaction (ECO 2 RR). The derived Cu nanosheets demonstrate much higher selectivity for C 2 H 4 production than commercial CuO derived Cu powder, with an optimum Faradaic efficiency of 56.2% and a partial current density of C 2 H 4 as large as 171.0 mA cm −2 in a gas diffusion flow cell. The operando attenuated total reflectance-Fourier transform infrared spectra measurements and density functional theory simulations illustrate that the high activity and selectivity of Cu nanosheets originate from the edge sites on Cu nanosheets with a coordinate number around 5 (4–6), which facilitates the formation of *CHO rather than *COH intermediate, meanwhile boosting the C C coupling reaction of *CO and *CHO intermediates, which are the critical steps for C 2 H 4 formation.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Ting Wang,Fuli Sun,Shoujie Liu,Guilin Zhuang,Benxia Li
Supported Cu single-atom (Cu-SA) catalysts have exhibited unique activity and selectivity in CO 2 reduction, but they generally suffer from the easy transformation of active Cu δ+ into inactive Cu 0 . Herein, porous TiO 2 supported Cu single atoms (Cu-SAs/TiO 2 ) photocatalyst was fabricated and dioxygen (O 2 ) enhanced photocatalytic CO 2 reduction performance of Cu-SAs/TiO 2 was investigated by in-situ characterizations and theoretical calculations. The results showed that both activity and stability of Cu-SAs/TiO 2 photocatalyst could be improved by feeding a small amount of O 2 (117.6 ppm) in the reaction system. The competitive electron transfer to O 2 on Cu-SAs/TiO 2 maintained dynamic stability of Cu δ+ active sites, and O 2 -derived *OOH species lowered the formation energy barrier of key intermediate *COOH as well as delivered *H species for accelerating intermediates protonation process. Total yield rate of CH 4 and CO reached 34.64 μmol·g cat ·h −1 for CO 2 photoreduction over Cu-SAs/TiO 2 after introducing 117.6 ppm O 2 , accompanied by enhanced durability.
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LANGMUIR
·
2023
·
IF 3.9
Jianmeng Wu,Zeying Yang,Jiaqi Xie,Peng Zhu,Jiajiao Wei,Renzhe Jin,Hui Yang
A decrease in CO2 emissions is urgently required in the present situation due to the fast growth of carbon dioxide (CO2) in the atmosphere, which has caused a series of global climate issues. This study used an impregnation–evaporation method to immobilize an amino functionalized ionic liquid [C2OHmim][Lys] on a chromatographic column filler GDX-103 and create a novel supported ionic liquid. The results showed that the supported ionic liquid with 60 wt % ionic liquid content had the best adsorption performance at 40 °C, and the CO2 adsorption isotherm showed that the adsorption capacity at 0.1 MPa was 1.29 mmol CO2/g sorbent, which was 6 times greater than the adsorption capacity of the pure carrier. The sample with 60% ionic liquid content has an adsorption capacity of 1.02 mmol CO2/g sorbent under the condition of CO2/N2 mixed gas with 10% CO2 content. This is 43 times greater than the adsorption capacity of the pure carrier, and its adsorption performance is stable after three adsorption and desorption cycles. Through the rich porous structure of GDX-103, the ionic liquid is effectively supported and dispersed, which expands the contact area between CO2 and ionic liquid and enhances the mass transfer of CO2. At the same time, CO2 can be chemically bound to the groups on the anion of ionic liquid and be immobilized, so it has a high selective adsorption capacity of CO2, which makes it a great alternative to traditional CO2 adsorbents.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
·
IF 5.2
Nan Kong,Huiling Du,Zhuo Li,Tong Lu,Siyu Xia,Ziwei Tang,Shijie Song
Metal-organic frameworks (MOFs), featuring semiconductor-like behavior, are promising for the photocatalytic reduction of CO 2 . While their practical application is hindered by the disadvantages of low charge migration efficiency and fast electron-hole pair complexation. In this paper, a simple solvothermal method was used to load NH 2 -UiO-66 onto the surface of MIL-101(Cr) to form a nano type II heterojunction double MOFs composite of NH 2 -UiO-66 @MIL-101. The results show that the heterostructure of NH 2 -UiO-66 @MIL-101 promotes the separation of photogenerated electron-hole pairs and accelerates the interfacial photogenerated electron transfer under light, and the NH 2 -UiO-66 @MIL-101 type II heterojunction exhibits higher activity for photocatalytic reduction of CO 2 compared with pure MIL-101(Cr) and NH 2 -UiO-66. In addition, the possible photocatalytic mechanism was further elucidated to demonstrate the increased photocatalytic activity of NH 2 -UiO-66 @MIL-101. This study provides effective insights for designing efficient MOFs photocatalysts for CO 2 reduction to enhance the photocatalytic activity for environmental protection and governance.
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GREEN CHEMISTRY
·
2023
·Vol. 25
·期 4
·1513-1521
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IF 9.8
Zhe Wang,Zhuo Li,Liying Liu,Peizhi Cao,Shupeng Li,Gang Kevin Li
Post-combustion carbon capture from fossil fuels for concentrated sources such as power plants is considered as one of the efficient ways to mitigate CO2 emissions. However, conventional adsorbents in physical adsorption processes have faced challenges in the presence of moisture in flue gases. Here, we successfully synthesized polypyrrole (PPy) adsorbent using Fenton's reagent and demonstrated that the filtrate could be recycled for the synthesis of PPy. The single-component gas-adsorption capacities of PPy were measured to obtain CO2, CH4, and N2 adsorption amounts of 16.73, 5.19, and 1.06 cm3 g−1 at 303 K and 101 kPa, respectively. Calculations by the IAST method demonstrated that PPy had excellent gas selectivities for CO2/N2 and CO2/CH4 of 46 and 4.0, which could be utilized for CO2 separation in flue gases and biogas. To simulate flue gas carbon capture, we investigated the dynamic adsorption capacity of PPy on CO2 in the presence of water vapor using a breakthrough device in the laboratory. The CO2 adsorption capacity was twice higher in moisture than in dry conditions, which was attributed to the presence of water vapor-formed hydrogen bonds that enhance its adsorption capacity through electrostatic and acid–base interactions of CO2 with PPy. This green and facilely synthesized polypyrrole adsorbent has great potential for carbon capture in high humidity flue gases.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
·
IF 5.2
Yangguan Chen,Jinrui Zhang,Haorui Liu,Xiaoqiong Wang,Shuixia Chen
Solid-amine adsorbents are promising CO 2 post-combustion adsorption materials to mitigate global warming. As one of the most important evaluation criteria, the CO 2 adsorption capacity of the adsorbent was determined by both kinetic and thermodynamic factors, while high temperature is good for mass transfer and low temperature is advantageous for equilibrium to move towards adsorption. In this study, surfactants were added into polyethylenimine (PEI) cryogel to enhance mass transfer and reduce the adsorption temperature, thereby promoting its adsorption capacity. With the addition of polyethylene glycol (PEG200), the CO 2 adsorption capacity reached a maximum value of 6.48 mmol/g at 65 °C, and the amine efficiency reached a maximum value of 0.52 mol C/mol N at 45 °C. Further characterization revealed that the addition of PEG not only enhanced the mass transfer, but also changed the chemisorption mechanisms, which were very similar to the effects of water. Besides, PEG would form hydrogen bonds with the PEI polymer network and showed stable regeneration capacity, thereby exhibiting a greater application potential.
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Menglin Wu,Jiupai Ni,Chengsheng Ni
In situ exsolution of nanoparticles has been reported to be an efficient path to optimize CO2 electrolysis performance. Herein, a Ce/Co co-doped SrFeO3-δ (SF) can achieve the co-exsolution of CeO2 and Co–Fe alloy in 5% H2 at 800 °C. A small amount (<10%) of Ce-doped SF cannot stabilize the perovskite structure in a reducing atmosphere. Sr0.9Ce0.1Fe0.9Co0.1O3 (10Ce10CoF) and Sr0.95Ce0.05Fe0.9Co0.1O3 (5Ce10CoF) as symmetric electrodes of solid oxide electrolysis cells showed an excellent electrolysis performance at 800 °C for CO2 electrolysis. The current densities of the cells with 5Ce10CoF and 10Ce10CoF reached 0.98 and 1.30 A cm–2 under a bias of 1.3 V after a 48 h durability test for CO2 electrolysis, respectively, and the performance difference, however, may be due to CeO2 being more easily exsolved from the 10Ce10CoF lattice. We also investigated the role of the exsolved CeO2 and oxygen vacancy (VO) in determining the CO2 electrolysis performance via theoretical calculation. In this work, we designed a novel strategy to achieve the exsolution of CeO2 and Co–Fe alloy via reduction treatment and showed an outstanding CO2 electrolysis performance.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Chaopeng Zhang,Chenguang Li,Wenjie Li,Xin Guo
Li 4 SiO 4 shows great promise for cyclic high-temperature CO 2 capture due to its excellent stability, high capacity, and low regeneration temperature. However, the practical application of Li 4 SiO 4 is mainly limited by the high cost of raw materials, particularly lithium resources. Additionally, the heavy use of lithium-ion batteries (LIBs) in developing renewable energy sources raises concerns about the disposal of many waste LIBs. This article synthesized Li 4 SiO 4 sorbent (BR-Li 4 SiO 4 ) using spent lithium cobalt oxide (LiCoO 2 ) cathodes and rice husk ash for CO 2 capture. Meanwhile, we also prepared R-Li 4 SiO 4 /P-Li 4 SiO 4 using commercial Li 2 CO 3 and rice husk ash/commercial crystalline SiO 2 as a comparison. The results show that the BR-Li 4 SiO 4 sorbent exhibited excellent CO 2 capture capacity and cycling stability at 675 °C, maintaining a stable capacity of 0.28 g/g under 100% CO 2 after 30 cycles. BR-Li 4 SiO 4 also demonstrated significantly reduced costs and a superior microstructure compared to R-Li 4 SiO 4 and P-Li 4 SiO 4 . Furthermore, the impact of a simulated flue gas containing 15% CO 2 and 10% H 2 O on Li 4 SiO 4 adsorption was investigated. It was found that the adsorption of CO 2 was decreased at low CO 2 concentrations, but the addition of 10% H 2 O showed a slight enhancement in CO 2 adsorption. Under a mixture of 15% CO 2 + 10% H 2 O (balanced with N 2 ), the maximum adsorption capacity of BR-Li 4 SiO 4 was 0.17 g/g, and its optimal adsorption temperature decreased by 50 °C to 625 °C compared to 15% CO 2 . Therefore, this study will provide valuable insights into the industrial application of Li 4 SiO 4 in CO 2 adsorption.
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