Advanced Science
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2025
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IF 14.1
Fengyi Zhong,Jianping Sheng,Chenyu Du,Ye He,Fengying Zhang,Yanjuan Sun,Ying Zhou,Fan Dong
Heterojunctions, known for their decent separation of photo-generated electrons and holes, are promising for photocatalytic CO 2 reduction. However, a significant obstacle in traditional post-assembled heterojunctions is the high interfacial barrier for charge transfer caused by atomic lattice mismatch at multiphase interfaces. Here, as research prototypes, the study creates a lattice-matched co-atomic interface within CsPbBr 3 -CsPb 2 Br 5 polytypic nanocrystals (113-125 PNs) through the proposed in situ hybrid strategy to elucidate the underlying charge transfer mechanism within this unique interface. Compared to CsPbBr 3 nanocrystals, the 113–125 PNs exhibit a remarkable 3.6-fold increase in photocatalytic CO 2 reduction activity (173.3 µmol −1 g −1 within 5 h). Furthermore, Kelvin probe force microscopy results reveal an increase in the built-in electric field within this lattice-matched co-atomic interface from 43.5 to 68.7 mV, providing a stronger driving force for charge separation and directional migration. Additionally, ultrafast transient absorption spectroscopy uncovers the additional charge carrier transfer pathways across this lattice-matched co-atomic interface. Thus, this unique co-atomic interface significantly promotes the interfacial electronic coupling and mitigates the charge transfer barrier, thus facilitating efficient charge separation and transfer. These insights underscore the importance of interfacial structure in heterojunction design and comprehending the intricate interplay between interface and carrier dynamics.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Xuewei Tu,Yutong Chen,Can Sun,Yang Hu,Shouxin Zhu,Jingyi Qu,Zhexiao Zhu,Shijie Zhang,Hui Zheng
The utilization of CO 2 as an economical C1 feedstock for the production of valuable fine chemicals is widely recognized as a green and environmentally friendly approach. In this work, iron/cobalt oxide nanowires (FCO@NWs) composites were synthesized by a simple, convenient and cost-effective hydrothermal process. The FCO@NWs catalyst demonstrated efficient CO 2 fixation with o -phenylenediamine to produce benzimidazole at atmospheric pressure and 150 ℃. After 12 h reaction, the conversion rate of o -phenylenediamine reached an impressive 98%, indicating the catalyst's high efficiency in CO 2 fixation process. Through orthogonal experiments, the optimal reaction condition was confirmed and the application of the FCO@NWs catalyst for various o -phenylenediamine derivatives by substrate expansion was screened. Notably, this catalyst exhibited easy recoverability and reusability without significant loss in catalytic activity even after five cycles of experimentation. This study presents a promising approach for fixing CO 2 into valuable benzimidazole derivatives and contributes some experience to sustainable chemistry.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Xianwei Fu,Ziyu Ma,Luoyu Liu,Sajjad Hussain,Qiuye Li,Dongwei Ma,Shilong Jiao
Electrochemical conversion of carbon dioxide into formic acid, which is one of the most economically viable chemicals, has been demonstrated as an efficient approach for closing the carbon cycle. However, it’s still challenging to reduce the overpotentials and increase the current densities for the future deployment of the CO 2 electrolysis technology. Here, we boost the intrinsic activity of the Bi-based electrocatalyst through the synergy of the enhanced charge transfer and mass transport process in the electrochemical reactions by generating an atomic disorder in the crystal lattices. The amorphous Bi-based quantum dots (a-BiQDs) serve as promising electrocatalysts toward formate production in a wide potential range with high Faradaic efficiency ( FE ) and energy efficiency ( EE ) in both the conventional H-cell and flow-cell, which is almost 5-fold enhanced in comparison with its crystalline counterpart. The maximum FEs of 94.44 % and 98.89 % are achieved at the potential of −1.0 V vs. RHE in the H-cell and flow-cell, respectively. Furthermore, long-term stability of more than 900 h is demonstrated in a two-electrode configuration. Combined molecular dynamics and first-principle calculations ascribe the remarkable activity toward formate production to synergistically accelerated mass transport and charge transfer kinetics during the electrocatalytic process. This work provides an effective approach for constructing electrocatalysts with high intrinsic activity, desired selectivity, and sufficient durability for large-scale deployment of CO 2 electrolysis technology.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2024
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IF 11.2
Mengyao Xu,Fei Liu,Shike Liu,Jun Ma,Mengqin Yao,Xiaodan Wang,Jianxin Cao
Metal-based catalysts are prevalent in the CO 2 hydrogenation to methanol owing to their remarkable catalytic activity. Herein, Ru/In 2 O 3 catalysts with different morphologies obtained by doping Ru into In 2 O 3 with irregular, rod-like, and flower-like morphologies are used for catalytic CO 2 hydrogenation to methanol. Results indicate that the flower-like Ru/In 2 O 3 (Ru/In 2 O 3 -F) exhibits higher catalytic performance than Ru/In 2 O 3 with other morphologies, achieving a 12.9% CO 2 conversion, 74.02% methanol selectivity, and 671.36 mg MeOH ·h −1 ·g cat −1 methanol spatiotemporal yield. Furthermore, Ru/In 2 O 3 -F maintains its catalytic stability over 200 h at 5 MPa and 290 °C. The promotional effect mainly stems from the fact that electronic structure of Ru can be effectively adjusted by modulating the morphology of In 2 O 3 . The strong interaction between atomically dispersed Ru and In 2 O 3 -F enhances the structural stability of Ru, inhibiting the agglomeration of the catalyst during the reaction process. Furthermore, density-functional theory calculations reveal that highly dispersed Ru atoms not only perform efficient and rapid electronic gain and loss processes, facilitating the catalytic activation of H 2 into H intermediates. It also enables the generated reactive H to rapidly overflow to the surrounding In sites to participate in CO 2 reduction. These findings provide a theoretical basis for the development of high-performance catalysts for CO 2 hydrogenation.
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Nano Today
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2024
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IF 13.2
Xiaoxiong Huang,Shengli Wu,Zhichang Xiao,Linjie Zhi,Bin Wang
We report a diatomic-site catalyst configuration constituted by Ni-N 3 and Bi-N 4 embedded in ultrathin nitrogenated carbon nanosheets (Ni/Bi-N-C) which showed dramatically improved activity and selectivity for the conversion of CO 2 to CO. Specifically, the catalyst exhibited high CO Faradaic efficiency (FE CO ) of above 90 % over a wide potential window from −0.76 to −2.22 versus reversible hydrogen electrode with the maximum CO partial current density up to 312 mA cm −2 in a flow cell, and coupled with robust durability. Ni/Bi-N-C-based membrane electrode assembly (MEA) device presented ultrahigh FE CO of 95.7 % at 750 mA and over 100 h of continuous operation without decay under constant current density of 100 mA cm −2 . Mechanistic studies and density functional theory calculations reveal that regulating the CO 2 RR catalytic performance via nearby Ni and Bi active sites can potentially break the activity benchmark of the single metal counterparts because the neighboring Ni and Bi active sites work in synergy to decrease the reaction barrier for the formation of *COOH and desorption of *CO. This work presents an efficient combination of two metal atomic sites which was designed by optimizing the interaction between the atomic sites and key reaction intermediates, resulting in the high-rate electrocatalytic CO 2 reduction.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Bingyuan Dai,Minxuan Wang,Hui Xu,Hongbing Zheng,Yongzheng Zhang,Cheng Ma,Jitong Wang,Wenming Qiao,Licheng Ling
The precise atomic-scale preparation of single-atomic active sites with unique coordination structures in electrocatalysts for the carbon dioxide reduction reaction (CO 2 RR), coupled with the elucidation of their mechanisms at the atomic level, remains a formidable challenge. In this manuscript, a simple one-pot synthesis method was adopted to successfully synthesize an O-doped Ni single-atom catalyst (Ni-NOG), characterized by a distinct Ni-N 2 O 2 symmetric coordination structure. The incorporation of Ni-O bonds alters the electronic configuration of the catalyst’s central atoms within the catalyst, thereby boosting both the catalytic selectivity and efficiency during CO 2 RR. The synthesized electrocatalyst exhibited outstanding performance in the CO 2 RR process, achieving a Faraday efficiency (FE) of 97.4 % at a potential of −0.8315 V versus to reversible hydrogen electrode (vs. RHE). Furthermore, the selectivity remained consistently above 95 % throughout a 98-hour stability test, surpassing the performance of most advanced catalysts currently available. Theoretical simulations demonstrate that the Ni-N 2 O 2 symmetric coordination structure shows a small activation barrier in the rate-limiting step, favoring the swift generation of intermediate species and demonstrating robust catalytic activity. This work not only offers a straightforward and approach method for the preparation of single-atom catalysts but also clarifies the pivotal role of O-element doping within the coordination environment in enhancing catalyst performance.
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Chemical Engineering and Processing-Process Intensification
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2025
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IF 3.9
Meng-Meng Du,Yuan-Cheng Wang,Bao-Chang Sun,Yong Luo,Liang-Liang Zhang,Guang-Wen Chu,Hai-Kui Zou
Carbonic anhydrase (CA) is a high-efficiency biocatalyst that significantly improves the absorption of CO 2 by tertiary amine. This work aims to investigate kinetics behaviors from the perspective of enzymatic reaction mechanism. The influences of the CA concentration, type of tertiary amines, pH, and temperature on the reaction rate between CO 2 and tertiary amine ( ν ) and catalytic activity of CA ( φ ) were first investigated in a stopped-flow device. Adding 50 g∙m⁻³ CA enhanced ν in tertiary amine solutions by a factor ranging from 22 to 42 at 298 K and pH=9.5, demonstrating its excellent catalytic performance. The ν increased with increasing CA concentration, pH, temperature, and tertiary amine's pK a. φ increased with the increase of CA concentration, as well as the decrease of temperature, pH, and tertiary amine's pK a. Proteomics analysis further revealed that conformational changes of the CA's secondary structure induced by high pH and temperature altered the expressions of the local active-site region and deactivated CA, ultimately leading to a decrease in φ . Additionally, the CA-catalysis kinetics equation accorded with the Michaelis-Menten model, with catalytic second-order rate constants on the magnitude of 10 7 . Overall, this work provides a guideline for its industrial application in the CO 2 capture process.
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APPLIED SURFACE SCIENCE
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2017
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IF 3.387
Degong Ding,Wenbo Lu,Ya Xiong,Xinglong Pan,Jianqiang Zhang,Cuicui Ling,Yonggang Du,Qingzhong Xue
In this paper, we presented a simple method to fabricate size-controlled La 2 O 2 CO 3 nanoparticle by annealing La(OH) 3 nanocrystallines in air atmosphere. The microstructures of the samples were analyzed by high resolution transmission electron microscope (HRTEM), X-ray diffraction (XRD) and scanning electron microscope (SEM). TEM images indicate that the La(OH) 3 precursors consists of uniform ellipsoids with width of 9–15 nm and length of 15–30 nm and La 2 O 2 CO 3 are spheroidal particles with size of 12–25 nm. XRD patterns indicate that La(OH) 3 nanocrystallines are hexagonal phase and transform to monoclinic La 2 O 2 CO 3 after annealing. And then, La 2 O 2 CO 3 nanoparticle is printed on an interdigital electrode as a sensing material for CO 2 detection. La 2 O 2 CO 3 sensor exhibits good cycle stability performance and fast response and recovery (53 s and 120 s) over the wide range of 300–5000 ppm CO 2 in air condition. In addition, we also investigate the effect of oxygen concentration in the background atmosphere on CO 2 response of La 2 O 2 CO 3 sensor. The CO 2 sensing mechanisms for La 2 O 2 CO 3 sensor can be attributed to the interaction of CO 2 with oxygen species on La 2 O 2 CO 3 surface including chemisorption, surface reaction and desorption process, which also can be used to explain other metal oxide based CO 2 gas sensor.
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CHINESE CHEMICAL LETTERS
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2016
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IF 1.947
Peng Cui,Xiao-Fei Jing,Ye Yuan,Guang-Shan Zhu
A novel porous aromatic framework, PAF-8, derived from tetraphenylsilane as basic building unit, was successfully synthesized via Friedel–Crafts alkylation reaction. This PAF material had high thermal stability as well as high surface area (785 m 2 g −1 ) calculated from the Brunauer–Emmett–Teller (BET) model. Meanwhile, PAF-8 possessed high performances in gas sorption and especially for CO 2 separation.
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ENERGY & FUELS
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2017
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IF 3.091
Ke Wang,Wei Li,Zeguang Yin,Zhongyun Zhou,Pengfei Zhao
A sodium chloride (NaCl) doping–hydration technique was used to modify the structure of Li4SiO4 to improve its sorption properties at a low CO2 concentration. X-ray diffraction, nitrogen adsorption, scanning electron microscopy, X-ray photoelectron spectroscopy, differential scanning calorimetry, and thermogravimetric analyses were conducted to characterize the compositions, textural characteristics, morphologies, chemical valence states, molten phases, and adsorption properties of the synthesized samples. Hydration and NaCl doping produced synergistic effects. On one hand, a small particle size and large specific surface area were obtained, significantly facilitating chemisorption processes. On the other hand, co-doped sodium and chlorine induced molten phases when absorbing CO2, noticeably decreasing CO2 diffusion resistance. Thus, the CO2 absorption rate and uptake were remarkably improved. Different amounts of NaCl also greatly affected the morphology and chemisorption properties of the sorbents. At the optimized NaCl concentration, the sorbent only required 3 wt % doping to attain a maximum sorption capacity of up to 34.2 wt %. Moreover, the high capacity was maintained after 10 sorption/desorption cycles.
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Journal of CO2 Utilization
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2017
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IF 4.292
Zhong Ying,Chaoyong Wu,Chao Zhang,Shan Jiang,Ruhui Shi,Haiyang Cheng,Bin Zhang,Yan Li,Fengyu Zhao
A series of polyureas were synthesized with CO 2 as the carbonyl building block, which consist of a hard segment of CO 2 -based oligourea and a soft segment of soluble polyether diamine. The hard segment was formed from 1,3-bis(3-aminopropyl) tetramethyl disiloxane with CO 2 , and the soft segment was obtained through polyaddition of polyether diamine with an extender agent. The Number-average Molecular Weight (Mn) and Weight-average Molecular Weight (Mw) were estimated by Gel permeation chromatography (GPC). The properties of the synthesized polyureas such as thermo-stability and the tensile strength were examined, and these properties could be adjusted by varying the molecular weight of polyether diamine and oligourea segments. The synthesized polyureas have an amorphous structure and presented satisfied thermo-stability (∼250 °C) and the high tensile strength (22.4 MPa).
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CHEMICAL ENGINEERING JOURNAL
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2016
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IF 5.31
Chuanwen Zhao,Yafei Guo,Weiling Li,Changsheng Bu,Xinye Wang,Ping Lu
K 2 CO 3 -modified silica aerogels (K 2 CO 3 /SG) were synthesized by the two-step sol-gel and wet impregnation method using K 2 CO 3 and tetraethoxysilane (TEOS) as starting materials and ethanol as solvent. CO 2 sorption behaviors of the sorbent were tested under ultra-dilute flue gas conditions of 20–60 °C, 1%CO 2 , 2%H 2 O and balanced N 2 with gas hourly space velocity (GHSV) of 4000 h −1 using a modified fixed-bed reactor. Experimental CO 2 uptakes of the sorbent under different temperatures were correlated to several kinetics models to study the kinetics performances. The effects of temperature, K 2 CO 3 loading, GHSV, H 2 O:CO 2 molar ratio and H 2 O pretreatment time on CO 2 sorption capacity and kinetics performances of the sorbent were further demonstrated. It is found that the two-step sol-gel and wet impregnation method could benefit the sorbent improved physical properties, superior surface characteristics and enhanced CO 2 sorption performances. Amongst various kinetics equations, the modified Avrami fractional kinetics model could well describe the CO 2 sorption process over K 2 CO 3 /SG. CO 2 sorption capacity decreases with the increase of temperature. With the increasing K 2 CO 3 loading, GHSV, H 2 O:CO 2 molar ratio and H 2 O pretreatment time, CO 2 sorption capacity increases first and then decreases. CO 2 sorption kinetics increases with the increasing temperature and H 2 O pretreatment time, while it decreases with the increasing K 2 CO 3 loading. CO 2 sorption kinetics keeps rather stable and then increases significantly with the increasing GHSV and H 2 O:CO 2 molar ratio.
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