Surfaces and Interfaces
·
2022
·
IF 6.137
Xianghui Zeng,Shuwen Li,Hui Chen,Wei Fang,Xuan He,Xing Du,Daheng Wang,Weixin Li,Zhaohui Huang,Lei Zhao
Transition metal doped 2D h-BN as a promising CO 2 adsorbent has recently been recognized, but the key to obtaining high-yield BN nanomaterials is to develop a simple synthetic method for practical industrial applications. Based on DFT calculation results, we found that Fe, Ni, and Co doping can significantly reduce the adsorption energy of h-BN for CO 2 . Accordingly, in-situ Fe, Ni, and Co doping of 2D BN nanosheets was achieved by “intermediate template” assisted molten salt method with sodium tetraborate and melamine as raw materials. During the synthesis process, the melamine was first transformed into two-dimensional C 3 N 4 (“intermediate template”) through controlled heating. The two-dimensional C 3 N 4 then acted as templates and carbothermic reducing agents to guide and promote the formation of two-dimensional BN. The Fe, Ni, and Co doped 2D BN nanosheets were synthesized at the temperature of 900 °C with up to 76 wt% yields, 1.77 times that of bulk BN prepared at the same experimental condition. In addition, Fe doped h-BN displayed a relatively high porosity with a specific surface area of 260.67 m 2 ·g −1 and its optimal CO 2 adsorption capacity could reach 7.69 cm 3 ·g −1 at 25 °C under atmospheric pressure in this research.
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
Nano Research
·
2024
·Vol. 17
·期 6
·5031-5039
·
IF 9.5
Li Wenxiang,Gao Shuo,Yang Chuanruo,Yang Juntao,Nisar Amjad,Xiang Guolei,Jin Junsu
In 2 O 3 is an effective electrocatalyst to convert CO 2 to formic acid (HCOOH), but its inherent poor electrical conductivity limits the efficient charge transfer during the reaction. Additionally, the tendency of In 2 O 3 particles to agglomerate during synthesis further limits the exposure of active sites. Here we address these issues by leveraging the template effect of graphene oxide and employing InBDC as a self-sacrificing template for the pyrolysis synthesis of In 2 O 3 @C. The resulting In 2 O 3 @C/rGO-600 material features In 2 O 3 @C nanocubes uniformly anchored on a support of reduced graphene oxide (rGO), significantly enhancing the active sites exposure. The conductive rGO network facilitates charge transfer during electrocatalysis, and the presence of oxygen vacancies generated during pyrolysis, combined with the strong electron-donating ability of rGO, enhances the adsorption and activation of CO 2 . In performance evaluation, In 2 O 3 @C/rGO-600 exhibits a remarkable HCOOH Faradaic efficiency exceeding 94.0% over a broad potential window of −0.7 to −1.0 V (vs. reversible hydrogen electrode (RHE)), with the highest value of 97.9% at −0.9 V (vs. RHE) in a H-cell. Moreover, the material demonstrates an excellent cathodic energy efficiency of 71.6% at −0.7 V (vs. RHE). The study underscores the efficacy of uniformly anchoring metal oxide nanoparticles onto rGO for enhancing the electrocatalytic CO 2 reduction performance of materials.
研究领域:
电化学
·
纳米材料
·
催化
·
能量转换
·
环境科学
✓ 已验证
DOI
高影响因子
CATALYSIS TODAY
·
2019
·
IF 4.888
Yunxia Zhao,Hui Ge,Yuanyuan Miao,Jiaxin Chen,Wei Cai
Metal-organic framework (MOF) materials have significant advantages for capturing CO 2 . To further improve the CO 2 adsorption performance of MOFs, a compound material of l -arginine modified graphene oxide (GO) with MOFs (MOF/GO-Arg) was synthesized. Introduction of amino acid-functionalized lamellar GO into MOF material not only generated new pores at their interface to improve the adsorption of the MOF but also promoted the CO 2 capture at low humidity. The structural and chemical properties of the parent components and composite materials were analyzed by X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), N 2 adsorption-desorption, thermal analysis and scanning electron microscopy (SEM). The dynamic CO 2 adsorption properties of the materials were compared under different temperatures, flow rates and humidities. Three kinetic models were used to fit the adsorption curves of the as-synthesized adsorbents under different conditions, and then the optimal dynamic model was determined. Since the reusability of the adsorbents is especially important for the use of these materials in practice, the CO 2 adsorption was repeated for 10 cycles under optimal temperature, flow rate and high humidity conditions.
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Deng Xianyu,Zhang Jianjun,Qi Kezhen,Liang Guijie,Xu Feiyan,Yu Jiaguo
Constructing S-scheme heterojunctions proves proficient in achieving the spatial separation of potent photogenerated charge carriers for their participation in photoreactions. Nonetheless, the restricted contact areas between two phases within S-scheme heterostructures lead to inefficient interfacial charge transport, resulting in low photocatalytic efficiency from a kinetic perspective. Here, In 2 O 3 /Nb 2 O 5 S-scheme heterojunctions are fabricated through a straightforward one-step electrospinning technique, enabling intimate contact between the two phases and thereby fostering ultrafast interfacial electron transfer (<10 ps), as analyzed via femtosecond transient absorption spectroscopy. As a result, powerful photo-electrons and holes accumulate in the Nb 2 O 5 conduction band and In 2 O 3 valence band, respectively, exhibiting extended long lifetimes and facilitating their involvement in subsequent photoreactions. Combined with the efficient chemisorption and activation of stable CO 2 on the Nb 2 O 5 , the resulting In 2 O 3 /Nb 2 O 5 hybrid nanofibers demonstrate improved photocatalytic performance for CO 2 conversion.
研究领域:
材料科学
·
光催化
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纳米技术
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
Ze Li,Youbin Zheng,Yuze Wang,Zhenjie Hao,Yuhui Huang,Rui Zhu,Dinghao Zheng,Ruixia Zhong,Liang Dong,Jianbing Zang,Pengfei Li,Zheng-Jun Wang
To address the kinetic limitations of CO2 desorption in the urea oxidation reaction (UOR), we develop a urotropine-induced strategy to engineer NiS–Ni3S2@g-C3N4 electrocatalysts. Urotropine, serving as both a structure-directing agent and g-C3N4 precursor, forms a dandelion-like architecture with narrowed columnar fluffs to maximize the surface area. The electronegativity difference between g-C3N4 and NiS–Ni3S2 induces local electron interactions, converting inactive sites to electron-enriched active sites and reducing adsorption energy barriers for CO2 desorption, the rate-limiting step. This catalyst exhibits outstanding UOR performance with a 1.24 V onset potential, 1.34 V to reach 100 mA cm−2, and 90% activity retention over 40 hours, while also demonstrating superior trifunctional activity rivaling IrO2 (OER: η10 = 90.9 mV) and Pt/C (HER: η10 = 13 mV). The urea electrolyzer requires only 1.26 V for 10 mA cm−2 with 48-hour stability. This work provides a breakthrough in designing efficient electrocatalysts through synergistic structural and electronic regulation.
✓ 已验证
产品关联
DOI
高影响因子
STAR Protocols
·
2022
·
IF 0
Xiaotong Li,Qian Liu,Jianghao Wang,Hao Bin Wu
Summary Heterostructured catalysts based on Cu and oxides are promising for the efficient conversion of CO 2 to multi-carbon products. In this protocol, we describe the fabrication and characterization of Cu/oxide heterostructured catalysts and the evaluation approach of electrochemical CO 2 reduction reaction (CO 2 RR) performance in an H-type cell. We also provide the details of in situ surface-enhanced Raman measurement and theoretical calculations. The protocol can be useful for constructing self-supported electrodes and assessing the CO 2 RR performance of as-fabricated electrodes. For complete details on the use and execution of this protocol, please refer to Li et al. (2022) .
研究领域:
材料科学
·
电化学
·
理论计算
✓ 已验证
DOI
FUEL
·
2021
·
IF 6.609
Zhige Zhang,Guofeng Zhao,Wenyang Li,Jiawei Zhong,Jun Xie
The efficient conversion of renewable biogas has attracted ever-increasing interest in past decades. Ni-CeO 2 -Al 2 O 3 supported on monolithic SiC-foam (denoted as Ni/CeO 2 -Al 2 O 3 /SCF) is designed and applied in biogas reforming. The monolithic Ni/CeO 2 -Al 2 O 3 /SCF catalysts were deeply characterized by XRD, ICP-AES, SEM, HR-TEM, CO 2 -TPD, etc. The cycle between CeO 2 -Al 2 O 3 and CeAlO 3 was verified by in-situ CH 4 /CO 2 -TPSR, and the catalytic role of CeAlO 3 in coke elimination and CO 2 activation was further confirmed. Due to the uniform distribution of Ni nanoparticles (NP S ) and the activation of CO 2 by CeAlO 3 , Ni/CeAlO 3 -Al 2 O 3 /SCF shows excellent catalytic stability to inhibit sintering and eliminate carbon deposition. At 900 °C and a gas hourly space velocity (GSHV) of 24000 mL g Cat -1 h −1 , excellent CH 4 /CO 2 conversion of 86/99% are initially achieved over Ni/CeAlO 3 -Al 2 O 3 /SCF catalyst, followed by slight decrease after 140 h, and remain basically stable for the next 260 h.
研究领域:
化学工程
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能源科学
·
催化材料
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Fei Guo,Dongsheng Li,Rui Ding,Jiaming Gao,Xuehua Ruan,Xiaobin Jiang,Gaohong He,Wu Xiao
Two-dimensional nanomaterials have the characteristics of high aspect ratio and high space utilization, which has huge potential advantages in gas separation. In this work, g-C 3 N 4 two-dimensional nanosheets with sieving pore structure were selected as templates and combined with ZIF-90 to construct a 0-dimensional/2-dimensional composite material ZIF-90@C 3 N 4 (ZCN). The complete two-dimensional g-C 3 N 4 nanosheets were stripped under acid etching conditions at 25 °C. ZIF-90 was distributed in an orderly manner on the two-dimensional nanosheets, and the nanosheets were spread out due to the growth of ZIF-90 to provide more free volume. The gas permeation experiment proved that the ZCN has a better CO 2 /N 2 separation performance. The ZCN/Pebax mixed matrix membrane (MMM) with the optimized 8.0 wt% ZCN loading showed an improved CO 2 permeability of 110.5 Barrer and a CO 2 /N 2 selectivity of 84.4, surpassing the Robeson upper bound (2008). The results demonstrated that the designed composite filler with 2D nanosheets is an effective strategy to enhance gas separation performance of MMMs and verified the application potential in gas purification industry.
研究领域:
材料科学
·
化学工程
·
气体分离技术
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yonghong Wang,Zhuo Jin,Xinru Zhang,Jinping Li
The incorporation of lamellar materials into polymer matrix can improve the gas separation performance of mixed matrix membranes (MMMs), which have great potential in chemical separation process. However, few intrinsic selectivity sites on MoS 2 sheets suppress further employment in the membrane separation. In this work, the vacancies and defects-containing MoS 2 sheets were prepared by high temperature oxidation and hydrothermal reaction in NaOH solution, and then L-cysteine-functionalized MoS 2 (Cys-MoS 2 ) was synthesized by a thiol-click chemistry reaction between S vacancies and thiol groups as confirmed by transmission electron microscope (TEM), Fourier-transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and N 2 absorption. After blending with polyether-block-amide (Pebax), the as-prepared MMMs showed outstanding mechanical properties as a result of the homogeneous dispersion of Cys-MoS 2 and hydrogen bonding between two phases as evidenced by attenuated total reflectance-FTIR, scanning electron microscope (SEM), thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC). The highest permeability of 297 Barrer accompanied with a CO 2 /N 2 selectivity of 120 was obtained for MMMs loaded with 1.5 wt% Cys-MoS 2 , which were enhanced by 206.2 % and 124.7 % over the pristine Pebax membrane, respectively. Meanwhile, this value was superior to that of the previously reported Pebax-based MMMs, transcending 2019 upper bound. The enhanced gas separation performance is due to the improved CO 2 adsorption selectivity by the vacancies and defects of Cys-MoS 2 , while the amine groups carrier enhanced CO 2 reactivity selectivity.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2025
·
IF 6.4
Qin Zhang,Jiancong Liu,Dongxu Wang,Chengxu Jin,Li Fang,Xingyu Li,Yingjie Jiang,Xin Wang,Chungui Tian
The construction of strong metal-support interaction (SMSI) between ultrasmall metal nanoparticles and semiconductor supports remains a pivotal challenge in developing high-performance photocatalysts for selective CO2 conversion. Herein, we propose a coordination-induced in-situ confinement strategy that synchronously achieves high dispersion of small-sized Ag nanoparticles (Ag NPs) and SMSI with ultrathin C3N4. Through melamine-mediated Ag-N coordination bonds, this approach orchestrates three synergistic effects: (1) Coordination-induced confinement of Ag NPs (~3.3 nm) via covalent Ag-N linkages, yielding an increase in active site density and stability compared to conventional Ag/C3N4; (2) Enhanced electron transfer from C3N4 to Ag, extending carrier lifetimes and suppressing charge recombination; (3) Interfacial electronic redistribution that promotes the generation of *COOH intermediates, steering the reaction pathway toward CO with high selectivity. Furthermore, the coordination-induced thermal condensation induces nitrogen vacancies in C3N4, which act as molecular traps to enhance CO2 adsorption capacity and synergize with Ag sites for efficient CO2 activation. As a result, the optimized catalyst exhibits a remarkable CO yield of 70.63 μmol·g-1·h-1 without the use of sacrificial agents, along with high selectivity (> 98 %) and excellent stability. This work establishes a universal paradigm for engineering metal-semiconductor interfaces through coordination chemistry, offering transformative insights into solar-driven CO2-to-fuel conversion technologies.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
·
2025
·
IF 5.6
Wenzhao Wei,Donggang Wang,Haibin Sun,Fangyong Yu,Xue Guo,Qiangqiang Hu,Yurun Feng,Hongli He,Xin Kong
Medium-entropy BaZr 0.1 Ce 0.5 Y 0.2 Dy 0.2 O 3-δ (BZCYD) electrolytes with a configurational entropy of 1.22 R are prepared by doping Dy element into low-entropy BaZr 0.1 Ce 0.7 Y 0.2 O 3-δ ( BZCY, 0.80 R). The entropy increasing strategy makes dramatically contribution to the improved chemical stability against CO 2 and H 2 O, and the relevant mechanism is clarified by the density functional theory (DFT). The BZCYD electrolyte shows stable phase composition and micro-structure after CO 2 heat treatment at 700 °C for 3 h and H 2 O treatment boiled for 3 h, while generation of impurities of BaCO 3 and Ba(OH) 2 accompanied by destroyed micro-structure are formed in the BZCY electrolyte under the same conditions. The total conductivity decay rates of BZCYD electrolyte after CO 2 heat treatment and H 2 O treatment are 44.1 % and 52.5 %, respectively, which exhibit significantly better than those of BZCY electrolyte (88 % and 74 %). According to the first-principles calculation, BZCYD electrolyte has higher CO 2 reaction energy barrier (5.21 eV) and H 2 O reaction energy barrier (7.30 eV), as well as lower CO 2 adsorption energy (−5.182 eV) and H 2 O adsorption energy (−0.742 eV), so it has better chemical stability. The peak power density of the anode-supported single cell with BZCYD electrolyte is 510 mW cm −2 at 700 °C in humid H 2 .
研究领域:
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Yaju Xue,Boxia Guo,Xiuling Ji,Bowen Li,Yuhong Huang
Glycine serves as a crucial element in basic metabolic processes and acts as a precursor in the production of numerous industrial chemicals. Here we developed a streamlined artificial cascade enzyme catalysis pathway for converting CO2 into glycine through improving the CO2 activation and employing direct C–C condensation. After the optimization of enzyme combinations and dose-dependent regulation, the integration of reduced nicotinamide adenine dinucleotide regeneration and ionic liquids were introduced and facilitated the construction of an artificial cascade ionozyme catalysis system. Consequently, the glycine yield reached a remarkable 17.87-fold increase compared to that of the initial reaction system. Additional molecular simulations further demonstrated that the ionozyme possessed enhanced structural stability and substrate affinity, as indicated by an increase in hydrogen bonds and a diminished interference from water molecules in protein–ligand binding. This innovative approach holds great promise for sustainable CO2 bioconversion to glycine and other valuable chemicals.
研究领域:
合成生物学
·
生物催化
·
二氧化碳利用
·
绿色化学
·
代谢工程
✓ 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）