查找使用阿拉丁产品的科研文献

Interfacial engineering on hierarchical ZrO2 nanozyme realizes efficient CO2 photoreduction

Shujie Liang,Yan Zhang,Jingxian Cong,Jiaxin Lv,Hong Deng

Designing and fabricating nanozymes with photoactivity for CO 2 reduction poses a significant challenge. Here, a hierarchically structured ZFs-tpyNi heterojunction nanozyme, comprising a terpyridine-based Ni complex supported on ZrO 2 nanoframes, has been created through an interfacial engineering strategy for efficient CO 2 reduction under visible light. Due to its unique structural and compositional advantages, ZFs-tpyNi demonstrates superior photocatalytic CO 2 -to-CO conversion compared to its counterpart of ZFs and tpyNi, achieving a CO yield of 18.2 µmol and a selectivity of 92.4 % with a high apparent quantum efficiency of 0.96 % in 3 h. These innovative catalysts also show excellent durability for at least eight cycles without a loss in performance, maintaining a remarkable structural stability with no obvious collapse of its framework and morphology. Systematic investigations reveal that ZFs-tpyNi heterostructures exhibit a high specific surface area advantageous for the effective loading of tpyNi and exposure of active sites. The robust ZFs framework, characterized by extensive porosity, prevents nanoparticle agglomeration and accelerates mass transfer during catalysis. Additionally, the spatially heterogeneous interface enables precise modulation of band alignment and bandgap dynamics in nanozymes, enhancing light absorption and promoting the generation and separation of photogenerated charge carriers. Consequently, the nanozyme demonstrates enhanced CO 2 adsorption and activation capabilities, leading to improved selectivity of catalytic products. This work aims at highlight the role of nanozyme catalysts in sustainable energy production.

Lanthanide single-atom catalysts for efficient CO2-to-CO electroreduction

Wang Qiyou,Luo Tao,Cao Xueying,Gong Yujie,Liu Yuxiang,Xiao Yusen,Li Hongmei,Gröbmeyer Franz,Lu Ying-Rui,Chan Ting-Shan,Ma Chao,Liu Kang,Fu Junwei,Zhang Shiguo,Liu Changxu,Lin Zhang,Chai Liyuan,Cortes Emiliano,Liu Min

Single-atom catalysts (SACs) have received increasing attention due to their 100% atomic utilization efficiency. The electrochemical CO 2 reduction reaction (CO 2 RR) to CO using SAC offers a promising approach for CO 2 utilization, but achieving facile CO 2 adsorption and CO desorption remains challenging for traditional SACs. Instead of singling out specific atoms, we propose a strategy utilizing atoms from the entire lanthanide (Ln) group to facilitate the CO 2 RR. Density functional theory calculations, operando spectroscopy, and X-ray absorption spectroscopy elucidate the bridging adsorption mechanism for a representative erbium (Er) single-atom catalyst. As a result, we realize a series of Ln SACs spanning 14 elements that exhibit CO Faradaic efficiencies exceeding 90%. The Er catalyst achieves a high turnover frequency of ~130,000 h − 1 at 500 mA cm − 2 . Moreover, 34.7% full-cell energy efficiency and 70.4% single-pass CO 2 conversion efficiency are obtained at 200 mA cm − 2 with acidic electrolyte. This catalytic platform leverages the collective potential of the lanthanide group, introducing new possibilities for efficient CO 2 -to-CO conversion and beyond through the exploration of unique bonding motifs in single-atom catalysts.

Indirect mineralization of CO2 using recyclable glycine with carbide slag

Xiongxiong Zhang,Mei Yang,Yonggang Sun,Yuanyuan Li,Yulong Ma,Wenxin Ji

The indirect mineralization of CO 2 by industrial solid waste is an essential process for CO 2 immobilization; however, many technical challenges remain to be overcome. In this study, carbide slag (CS), a type of industrial solid waste, was used as a raw material for the indirect mineralization of CO 2 using glycine. In the extraction stage, the ion extraction efficiency of Ca significantly increased to 68.5 % due to the formation of a chelate between glycine and Ca, which enhanced Ca dissolution. Analysis of the mineralization process revealed that glycine was recycled after absorbing CO 2 , leading to increased CO 2 absorption capacity because of the high alkalinity of the extract solution. Furthermore, there was a synergistic effect between CO 2 absorption and the Ca precipitation reaction. This synergistic effect increased the reaction rate of mineralization and enhanced its efficiency. As a result, the Ca precipitation reaction was largely complete within 5 min, and the mineralization efficiency was enhanced to 93 %. Furthermore, the recirculation (indirect mineralization) results showed that the Ca extraction and mineralization efficiencies remained constant during each cycle. Most importantly, glycine could be regenerated automatically during the cycle, which proved that the cyclic indirect mineralization process could operate stably.

Mitigating Asphaltene Deposition in CO2 Flooding with Carbon Quantum Dots

Qi Liu,Yangwen Zhu,Hang Ye,Haiying Liao,Quanqi Dai,Michelle Tiong,Chenggang Xian,Dan Luo

Carbon capture, utilization, and storage (CCUS) technology has emerged as a pivotal measure in mitigating global climate change. Notably, CO2-EOR is esteemed for its dual function of sequestering CO2and enhancing oil recovery. However, this process presents challenges related to asphaltene deposition during CO2flooding, leading to reservoir damage, such as pore plugging. This study systematically manipulated the factors inducing CO2-induced asphaltene deposition, elucidating the mechanisms and magnitudes of asphaltene precipitation. Additionally, the study investigated the efficacy of carbon quantum dots (CQDs) in mitigating asphaltene deposition. Experimental findings indicated a positive correlation between asphaltene deposition and level of asphaltene content, CO2injection ratio, and temperature. Moreover, with an increase in experimental pressure, the asphaltene deposition rate demonstrated an initial increase followed by a subsequent decline. Leveraging their favorable compatibility with asphaltene, CQDs effectively suppressed the aggregation behavior of asphaltene. In the presence of CQDs, the onset of asphaltene precipitation was delayed from 45 V% to 55 V%, with the highest inhibition rate reaching approximately 36% at an optimal CQD concentration of 20 mg/L. This study proposes a novel approach to address asphaltene deposition issues in CO2-EOR processes, contributing to the enhancement of recovery rates in low-permeability reservoirs.

Molecular scale insights into CO2 hydrate growth regulated by surfactant

Xingbo Li,Liangyue Jiang,Zhe Zhang,Shengyang Tao,Yongchen Song

Carbon dioxide hydrate is an efficient technology for carbon dioxide capture and storage, and its growth is a complex process involving multiple phases and components. Typically, the nucleation and growth of hydrates require the introduction of surfactants to improve interfacial compatibility. In this study, we designed and synthesized two new surfactants (QC 12 PyBr and QAC 12 Et 3 Br), both deploying fluorescent group (quinoline) for the hydrophobic end. To enhance the weak interaction with H 2 O molecules, pyridine and triethylamine are introduced as the hydrophilic end with QC 12 PyBr and QAC 12 Et 3 Br respectively. This design endowed the surfactants with optical activity (UV illumination) while maintaining their original amphiphilic properties. The effects on hydrate growth are explored by molecular dynamics simulations, which provide molecular scale insights into CO 2 hydrate growth regulated by surfactant from the perspectives of CO 2 aggregation morphology, surfactant conformation, as well as weak intermolecular interactions, respectively. The results indicate that the spherical morphology with higher interface curvature of CO 2 aggregation is more favorable for hydrate growth. DFT calculations show that the differences in intermolecular interactions between hydrophilic groups and H 2 O molecular lead to different surfactant spatial conformations at the gas–liquid interface. Additionally, a combination of simulation and experimental methods is employed to further verify the feasibility of the surfactants designed in this study, thus confirming that the synthesized surfactant possesses the ability to effectively regulate hydrate growth for CO 2 storage while providing a new method for monitoring hydrate film growth based on the fluorescence activity.

Oxygen vacancies on CuGa2 catalysts enhance CO2 reduction to CO

Jiangfeng Mou,Jin Hu,Tianyou Chen,Kaizhao Wang,Kaijun Wang,WeiJun Zhang,Shuai Wu,Jin Shi,Pengchong Zhao

Electroreduction of CO2 into fuels and valuable chemicals is an effective way to alleviate the greenhouse effect. However, CO2 is chemically inert owing to the highly stable CO bond. Thus, CO2 activation is recognized as a critical reaction step in the process. As electron transfer to CO2 is commonly accepted as the key step during the activation of CO2, it is crucial to engineer the electronic properties of catalysts to enhance their performance in the electrochemical reduction of CO2. Herein, we prepared a CuGa2 catalyst with oxygen vacancies (O–CuGa2) to effectively improve product selectivity. O–CuGa2 exhibited a current density of 32.9 mA cm−2 with a faradaic efficiency of 82.6% for CO production in a tetrabutylammonium chloride/acetonitrile (Bu4NCl/AN) electrolyte, which is 2.5 times higher than that exhibited by CuGa2. XPS and EPR results indicated that OV concentration in O–CuGa2 is much larger than that in the CuGa2 catalysts. The results of electrokinetic studies indicated that the introduction of OVs facilitate electron transfer to CO2.

CO2-switchable vesicles-network structure transition and drug release property

Wenmeng Duan,Xianwu Jing,Jiang Tan,Minmin Tao,Lu Wang,Hongsheng Lu

Dopamine-modified Highly Dispersed ZIF-8 to Promote CO2 Absorption

Donglin Jiang,Yuchen Zhou,Mengfan Du,Zezhi Chen,Huijuan Gong

Graphical The modification of ZIF-8 with dopamine results in a large amount of hydrophilic and CO 2 friendly groups introducing into the ZIF-8 molecules, and the structure and specific surface area of ZIF-8 is also improved. These factors lead to an improvement performance of ZIF-8 in the catalytic CO 2 absorption in water and alkaline solutions. CO 2 capture technology has been widely used to reduce CO 2 emissions, resulting in a variety of capture methods and materials. Among them, the more widely used is the chemical absorption method. However, the chemical absorption method has problems such as high energy consumption and slow absorption rate. In order to solve the above problems, we prepared an effective catalyst to improve the CO 2 absorption rate. ZIF-8 and hydrophilic ZIF-8-DA were prepared by in situ synthesis under ambient conditions. The catalytic effect of the hydration reaction of ZIF-8 and ZIF-8-DA was tested using CO 2 absorption regeneration experiments under aqueous and alkaline conditions, respectively. The results showed that the synthesized catalysts could significantly enhance the CO 2 absorption in water and alkaline solution. The addition of 0.1 wt % of ZIF-8 in alkaline solution increased the average CO 2 absorption by 1.80–15.84 %, respectively, while the addition of 0.1 wt % of ZIF-8-DA increased the CO 2 absorption by 7.01–25.36 %. In addition, both catalysts had excellent reusability and maintained high performance even after five absorption and regeneration cycles. Polymer dispersibility index (PDI) results showed that ZIF-8-DA dispersed more uniformly in aqueous solution.

CO2 hydrogenation to methanol over the copper promoted In2O3 catalyst

Rui Zou,Chenyang Shen,Kaihang Sun,Xinbin Ma,Zhuoshi Li,Maoshuai Li,Chang-Jun Liu

The metal promoted In 2 O 3 catalysts for CO 2 hydrogenation to methanol have attracted wide attention because of their high activity with high methanol selectivity. However, there was still no experimental confirmation if copper could be a good promoter for In 2 O 3 . Herein, the Cu promoted In 2 O 3 catalyst was prepared using a deposition-precipitation method. Such prepared Cu/In 2 O 3 catalyst shows significantly higher CO 2 conversion and space time yield (STY) of methanol, compared to the un-promoted In 2 O 3 catalyst. The loading of Cu facilitates the activation of both H 2 and CO 2 with the interface between the Cu cluster and defective In 2 O 3 as the active site. The Cu/In 2 O 3 catalyst takes the CO hydrogenation pathway for methanol synthesis from CO 2 hydrogenation. It exhibits a unique size effect on the CO adsorption. At temperatures below 250 °C, CO adsorption on Cu/In 2 O 3 is stronger than that on In 2 O 3 , causing higher methanol selectivity. With increasing temperatures, the Cu catalyst aggregates, which leads to the formation of weak CO adsorption site and causes a decrease in the methanol selectivity. Compared with other metal promoted In 2 O 3 catalysts, it can be concluded that the catalyst with stronger CO adsorption possesses higher methanol selectivity.

Cu Nanocrystals on Carbon Nitride for the CO2 Reduction Reaction

Pengxuan Wu,Wanbing Ma,Yuxin Ge,Jinbao Xu,Minglei Lu,Xia Li,Liang Ma,Song Bai,Tiejun Wang

A facile one-step method was developed to promote the carbon dioxide reduction reaction (CRR) activities to form the C2 products (C2H4 and C2H5OH) via the capping agent and organic solvent-free involvement of copper (Cu) on graphitic carbon nitride (GCN). By tuning the using amount of the Cu precursor, Cu-GCN-0.2 exhibited a total Faradaic efficiency (FE) of more than 86.69 ± 0.73% for the C1 species (CO, CH4, HCOOH) and C2 species (C2H5OH, C2H4) as the CRR products when the electrolysis was carried out at an overpotential of 0.7 V (vs RHE) even after 12 h electrocatalysis and at a ratio of about 1:1 for C2/C1. Further investigation confirms that the enhanced CRR activities can be ascribed to three aspects: Firstl’y, smartl’y regulation of the Cu involvement during the synthesis of GCN created the CRR active site, which enables more CO2 to be adsorbed and activated at a lower overpotential to participate in the C–C couple procedures. Secondly, the neglected HER active site was formed when Cu was involved, which enables the well-maintained proton generation and adsorption activities for the proton-coupled electron transfer procedures, leading to the promoted C2/C1 ratio. Thirdly, the decreased electronic resistance accelerates the electronic transfer speed, which enables a faster reaction rate and a promoted long-term durability performance. This research provides a facile method for the rational construction and preparation of the electrocatalyst toward large-scale utilization in sustainable conversion and application.

Electrocatalytic CH4 production from CO2 by SiO2-induced amorphous CuOx

Jianing Mao,Guanghui Feng,Xiao Dong,Ziran Xu,Bingbao Mei,Yiheng Wei,Xiaohu Liu,Guihua Li,Shoujie Li,Yanfang Song,Fei Song,Wei Wei,Wei Chen,Zheng Jiang

CH 4 , as an important clean fuel and hydrogen carrier, its production from CO 2 driven by renewable energy could simultaneously achieve energy supply, CO 2 emission reduction, and renewable energy consumption, which is of great significance. Electrocatalytic CH 4 production relies on high-valence Cu species for realizing multielectron reduction, while facing inadequate performance stability due to the reconstruction tendency of Cu. Herein, an amorphous CuO x -SiO 2 catalyst (amorCuO x -SiO 2 ) is synthesized via an electrostatic interaction strategy to construct stable Cu 2+ active sites for efficient electrocatalytic CH 4 production. AmorCuO x -SiO 2 shows a good reconstruction resistance during electroreduction, confirmed via X-ray absorption spectroscopy studies, endowing a 63.7% CH 4 faradaic efficiency at 500 mA cm −2 , which is 7.8 folds of crystalized CuO x -SiO 2 (crysCuO x -SiO 2 ). Theoretical calculations revealed that stable Cu 2+ active sites enhanced *CO adsorption and were more susceptible for further hydrogenation, thus promoting the CO 2 -to-CH 4 conversion. Our findings provide a feasible strategy for developing reconstruction-resistant electrocatalysts for advanced CH 4 production performance.

Electrocatalytic CO2 reduction promoted by catalyst-bound proton-abstracting ligands

Nana Zhou,Yurong Yin,Baojuan Luo,Yongxin Fu,Xiaoxun Ma,Chengyi Dai

The electrochemical CO 2 reduction reaction (eCO 2 RR), which is well suited for reducing atmospheric CO 2 levels and generating clean energy. Water is the main proton source in the electrochemical reduction process. However, water features a high dissociation energy barrier, and most protons are involved in HER, so that only a small amount of H + is used in the CO 2 reduction reaction. Herein, we reveal that appropriately chosen ligands on the catalyst surface can abstract protons from water, store them, and transfer them to CO 2 to promote the formation of COOH and improve the proton utilization efficiency of the eCO 2 RR. Moreover, the activity of the ligand complexed protons is shown to be lower than that of free ones and thus result in HER inhibition our ligands with different pK a values (i.e., proton release capacities) are used to functionalize ZnO, and the plot of pK a vs. the FE CO exhibits a volcano shape. Overly small pK a leads to the combination of abundant protons with each other and the dominance of the HER, whereas overly large pK a does not promote the utilization of H + by CO 2 . Ligands with suitable pK a can properly bind and release protons, which is conducive to the formation of *COOH, thus accelerating eCO 2 RR. In particular, mercaptobenzoic acid (MBA) considerably enhances catalytic activity because of its moderate pK a (FE CO  = 90 %, which is 2 times higher than the FE CO of unmodified ZnO, and j CO is nearly 5 times higher). In situ infrared spectroscopic analysis proves that the above ligand can abstract protons from H 2 O and then release them, promoting the dissociation of H 2 O. Theoretical calculations show that pK a affects the ability of ligands to abstract and release protons.