ACS Applied Nano Materials
·
2025
·
IF 5.5
Xudong Zhao,Shuibo Wang,Hua Li,Yushi Wei,Yiming Li,Haocheng Li,Hongbo Yu,Kaijie Li,Haotian Li,Hongfeng Yin
Preventing nanoparticle migration and agglomeration on the surface of supported heterogeneous catalysts, especially at tailored bimetallic sites, poses a significant challenge. The reverse water–gas shift (RWGS) reaction is considered a promising route for converting CO2 into CO, an essential feedstock for industrial chemical production. Herein, a core–shell nanostructure anchoring on the surface was developed, which consists of a PtFe bicomponent core (∼2.6 nm) and a nitrogen-doped carbon nanoshell (∼1.3 nm). This structural design enhances the CO2 adsorption saturation, weakens the CO adsorption strength, and promotes hydrogen spillover. This PtFe core–shell material (Pt/Fe = 1:1) demonstrates an elevated reaction rate of 12.58 molCO2 gPt–1 h–1, with nearly 100% CO selectivity at 450 °C and atmosphere pressure. The activity is 5.1-fold higher than that of the Pt nanoparticle, attributed to the tuned geometric and electronic properties. The nitrogen-doped carbon nanoshell preserves the core–shell morphology at a high temperature. Moreover, the in situ experiments reveal the H-assisted dissociation/activation of the CO2 pathway for RWGS. The integration of the bimetallic synergy and core–shell structure is a potent strategy for thermal catalytic processes.
研究领域:
材料科学
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催化化学
·
环境科学
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DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Shiwei Liang,Xingcan Qian,Tianxin Zhang,Guiqin Song,Bing Wang,Yongsheng Yang,Xiansong Yang,Danyang Lin,Xiu He,Long Zou
Regulating the valence states and composition of a catalyst surface allows a precise control of the electronic structure, enabling enhanced catalytic activity and improved detection sensitivity of sensors. Herein, an accurate quantification of hydrogen peroxide (H 2 O 2 ) has been achieved using a colorimetric and electrochemical sensing platform based on the catalytic activity of cobalt@nitrogen-doped carbon (Co@NC) nanocatalysts in acidic (pH 3.6) and neutral (pH 7.4) environment. A series of Co@NC samples were synthesized by electrospinning and subsequent calcination, where Co@NC-3 with a high Co 3+ /Co 2+ potential (1.92 V) facilitates the direct oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) under acidic conditions. In the presence of H 2 O 2 , TMB oxidation was inhibited due to cyclic reactions involving oxidized TMB and H 2 O 2 on the Co@NC-3 surface, with an associated loss of the blue coloration that is detectable by the naked eye and is quantified by UV–vis spectrometry with a detection limit of 40.5 μM. Moreover, the Co 3+ /Co 2+ redox cycle on the surface of the Co@NC-3 modified glassy carbon electrode resulted in enhanced electrocatalytic H 2 O 2 reduction in a neutral phosphate buffered saline, where the amperometric currents exhibited a linear response to H 2 O 2 concentration over the 0.05–27.6 mM range with a detection limit of 3.16 μM, and an enhanced sensor sensitivity (991 μA mM −1 cm −2 ). The proposed Co@NC-3 detection system has been applied to real-time measure the concentration of H 2 O 2 released from HeLa cells. The colorimetric and electrochemical sensing analysis delivers reliable detection efficiency with important practical applications in clinical analysis and diagnosis.
研究领域:
生物医学工程
·
分析化学
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DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Yi-Ming Gu,Ya-Hui Wang,Sheng-Sheng Zhao,Hong-Jun Fan,Xiao-Wei Liu,Zhiping Lai,Shu-Dong Wang
Carbon capture from flue gases is one of the crucial routines for reducing current CO 2 emissions and mitigating the greenhouse effect. Metal-organic frameworks (MOFs) have received a lot of interest as efficient solid adsorbents for CO 2 /N 2 separation in flue gas treatment. However, many MOF materials are susceptible to the presence of water vapor, which has a significant impact on their adsorption efficacy and moisture stability. Here in this work, we reported two pillar-layered Zn-MOFs with N -donors, i.e., Zn 2 (TRZ) 2 (Fuma) and Zn 2 (TRZ) 2 (BDC), which demonstrated high CO 2 uptakes (3.92 and 1.52 mmol/g) and CO 2 /N 2 (132 and 20.5) adsorption selectivities at 298 K and 101 kPa, among the best comprehensive results reported by far. After seven days of exposure to a 100 % RH environment, it was found that, the Zn-N pillar contributes to the robust structure of MOFs . Furthermore, in-depth theoretical calculations indicated the guest-framework interactions, and dynamic sorption tests confirmed high working capacities (2.78 and 1.14 mmol/g), sufficient water stability and remarkable cycling performance of the studied MOFs under humid ambient conditions. We believe this work provides a routine to prepare robust and promising candidates to address the challenge in carbon capture under humid conditions.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
RENEWABLE ENERGY
·
2026
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IF 9.1
Huage Lin,Weiyan Su,Yihan Tang,Jiaxiang Zong,Guangyu Wu,Weinan Xing
The scalable synthesis of green chemical fuels via artificial photosynthesis represents a cornerstone strategy for buffering intermittent renewable energy and advancing global carbon neutrality. However, the practical engineering deployment of this technology is severely constrained by suboptimal solar-to-fuel conversion efficiencies at the catalytic interface. Herein, a tubular S-scheme Co 2 (OH)PO 4 @CN (CoHP@CN) heterojunction was fabricated via a pre-coordination-mediated in-situ growth strategy to facilitate solar energy harvesting. Characterizations reveal that a directional internal electric field (IEF) drives an S-scheme charge pathway, significantly reducing transfer resistance while preserving strong redox capabilities. Benefiting from these kinetic features, the heterojunction delivers exceptional solar fuel production performance, achieving a CO yield of 383.40 μmol g −1 (over 4 h) and H 2 evolution of 4657.40 μmol g −1 (within 2 h). This study underscores the power of precise interface engineering in modulating charge dynamics, offering practical insights for scalable solar-to-chemical energy storage and renewable energy deployment.
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高影响因子
ACS Applied Materials & Interfaces
·
2026
·Vol. 18
·期 32
·43974-43984
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IF 7.8
Zhang Chuyi,Sun Zhi,Kong Weiqian,Wu Wenzhuo,Zheng Xiaoli,Xu Qun
The enhancement of photocatalytic efficiency is limited by exciton dynamics, where photogenerated electrons and holes rapidly recombine due to strong Coulomb attraction. The manipulation of electron spin, involving the control of electron spin and spin states, has emerged as a promising strategy to improve photocatalytic performance via spin-polarization-facilitated charge separation. In this work, we demonstrate a spin-polarization effect achieved by treating ZnSn(OH) 6 (ZHS) with supercritical CO 2 (SC CO 2 ), which accelerates exciton dissociation and spin-dependent electron migration, thereby enhancing the efficiency of photocatalytic CO 2 reduction to CO. Mechanistic investigations reveal that SC CO 2 treatment induces oxygen vacancies in ZHS, generates spin-polarized electrons, and selectively exposes highly active {111} crystal facets. Experimentally, it reveals that the oxygen vacancies, together with adjacent hydroxyl groups, construct frustrated Lewis pairs (FLPs). Through enhanced quantum spin exchange interactions (QSEIs), the recombination of photogenerated charge carriers is significantly suppressed, and then their lifetime is prolonged, and CO 2 adsorption and activation are simultaneously enhanced. It was found that, under treatment at 16 MPa of SC CO 2 , the CO production rate of ZHS reaches 144.82 μmol·g –1 ·h –1 , which is 29.37 times that of the untreated sample. Therefore, this study demonstrates that manipulating spin-polarized electrons in photocatalytic semiconductors is an effective strategy to boost CO 2 RR efficiency, offering new insights for the design of efficient spin-dependent photocatalysts toward solar energy conversion.
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高影响因子
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2026
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IF 4.4
Si Liu,Zixuan Xu,Qun Liao,Xingxing Zheng,Xionghui Fu,Yuanming Zhang,Yi Zhu
Co₃O₄/TiO₂ achieves a CH₄ yield of 34.8 μmol g −1 h −1 with 82.4% selectivity. • Ti–O–Co bonds serve as charge transfer channels in Co₃O₄/TiO₂. • Co 2+ /Co 3+ redox couples stabilize *CO intermediates and facilitate PCET. • Electron transfer promotes Co electron enrichment for *CO stabilization. • Synergistic electron transfer and proton supply promote selective CO₂ methanation. Value-added conversion of CO 2 using solar energy is a sustainable strategy to address the energy crisis and environmental issues simultaneously. In this work, Co 3 O 4 /TiO 2 composite photocatalysts were successfully prepared by a hydrothermal method. The optimized Co 3 O 4 /TiO 2 achieves a CH 4 yield of 34.8 μmol·g −1 ·h −1 with 82.4% selectivity. The enhanced catalytic activity is ascribed to interfacial Ti-O-Co bonds that facilitate electron transfer toward Co sites, thereby modulating the Co 2+ /Co 3+ electronic environment and creating relatively electron-rich Co sites for *CO stabilization, while the Co 3 O 4 component facilitates the proton-coupled electron transfer (PCET) process toward CH 4 formation. This study provides a practical strategy for promoting the value-added photocatalytic conversion of CO 2 using multivalent transition metal oxide composite photocatalysts. Co 3 O 4 /TiO 2 enables highly selective photoreduction of CO 2 into CH 4 . Ti-O-Co bonds serve as pathways transferring photogenerated electrons from TiO 2 to Co sites. The electron-rich Co centers act as active sites to stabilize *CO intermediates. Meanwhile, Co 3 O 4 promotes water oxidation and maintains sufficient proton supply, synergistically facilitating CH 4 production. Download: Download high-res image (200KB) Download: Download full-size image
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
·
IF 13.2
Huiyuan Cheng,Jingwei Hu,Shaoke Bu,Yushuang Shi,Guangping Lei
The escalating atmospheric concentration of CO 2 has intensified the demand for efficient carbon capture technologies. Here, an innovative composite adsorbent, Cu-Salophen@Cu-BTC, was successfully synthesized via an in-situ encapsulation strategy to enhance the selective adsorption of CO 2 from CO 2 /N 2 mixture. The incorporation of Cu-Salophen into the Cu-BTC framework was confirmed through XRD, ICP-OES, and FT-IR analyses. The composite exhibited a notable improvement in CO 2 uptake capacity, reaching 8.14 mmol g −1 (273 K) and 4.63 mmol g −1 (298 K) at 100 kPa, representing increases of 11.81% and 12.11%, respectively, compared to pristine Cu-BTC. Moreover, the CO 2 /N 2 separation performance was enhanced by 23.44% (273 K) and 36.06% (298 K). GCMC simulations revealed that the superior performance arises from the synergistic effects of additional adsorption affinities of CO 2 and real-time pore size regulation enabled by the mobile Cu-Salophen molecules. The composite also demonstrated excellent recyclability and improved water stability, underscoring its potential for industrial post-combustion CO 2 capture.
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高影响因子
Science China-Chemistry
·
2026
·
IF 9.8
Wang Nan,An Tinghui,Li Jiaqi,Wang Yuhao,Xiang Dong,Cai Kedi
Cu-based electrocatalysts are promising for the electrocatalytic CO 2 reduction reaction (eCO 2 RR) to realize valuable chemicals production. Here, a Mg-doped Cu based electrocatalysts via transient CO 2 pulsed laser (L 4 -Mg/Cu x O) was synthesized for highly selective eCO 2 RR to ethanol (C 2 H 5 OH). The synergistic effect of Mg-doping and transient CO 2 pulsed laser irradiation enables excellent eCO 2 RR performance, realizing Faradaic efficiencies (FE) of 52.2% and 74.1% for C 2 H 5 OH and C 2 products under a high current density of 298.9 mA cm −2 , respectively. Operando Raman spectroscopy and DFT simulations results confirm that Mg-doping strategy suppresses the hydrogen evolution reaction (HER), enhances CO adsorption, elevates local pH and accelerates H 2 O dissociation, which could be beneficial for promoting OC–CO coupling and proton supply in eCO 2 RR. Furthermore, Mg incorporation induces electron delocalization in which electron accumulation on the C atom of *CHCOH intermediate and its enhanced p-d orbital coupling with Cu interface, which stabilizes the C–O bond from breakage and selectively favours the C 2 H 5 OH pathway, thus decoupling the selectivity between C 2 H 5 OH and ethylene. When employed in Li-CO 2 batteries, L 4 -Mg/Cu x O delivers 20480 mAh g −1 discharge capacity and cycling stability over 187 cycles. This work presents a universal strategy for regulating eCO 2 RR selectivity through precise laser energy delivery, demonstrating significant potential for renewable energy conversion and storage.
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高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2026
·
IF 4.4
Li Shiheng,Li Wei,Zhang Baojing,Wang Xiaohong,Feng Peizhong
The widespread application of solid amine adsorbents is hindered by the cost and complexity of synthesizing porous supports, which typically require templating agents and energy-intensive calcination. Herein, we report a facile and mild method to fabricate nanoporous silica, involving CO 2 -induced gelation of low-cost sodium metasilicate, followed by freeze-drying. The obtained silica support exhibits a pore volume of 1.22 cm 3 /g and a specific surface area of 378.5 m 2 /g, which is suitable for amine loading. After impregnation with tetraethylenepentamine, the optimal adsorbent with 50% tetraethylenepentamine loading delivers a competitive CO 2 adsorption capacity of 3.48 mmol/g at 70 °C. More importantly, it demonstrates exceptional cycling stability, maintaining 3.37 mmol/g of CO 2 adsorption capacity after 10 cycles, with a minimal capacity loss of only 0.3% per cycle. This work demonstrates that high-performance adsorbents can be fabricated via a drastically simplified process, offering an amenable to scale-up and economically attractive strategy for practical CO 2 capture. Graphical abstract This paper presents an innovative and template-free synthesis of a high-performance solid amine adsorbent for CO 2 capture. The method innovatively utilizes CO 2 as both a reactant and an in-situ porogen to fabricate nanoporous silica from sodium silicate via a simple one-pot gelation process, entirely bypassing the need for templating agents and energy-intensive calcination. After freeze-drying and tetraethylenepentamine (TEPA) impregnation, the optimal adsorbent with 50% TEPA loading achieves a high CO 2 capacity of 3.48 mmol/g at 70 °C and demonstrates exceptional cyclic stability with 96.8% capacity retention after 10 cycles. This study provides a simplified, cost-effective, and scalable pathway for practical carbon capture applications.
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DOI
高影响因子
Journal of CO2 Utilization
·
2017
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IF 4.292
Lijun Zhao,Haiyang Cheng,Tong Liu,Yan Li,Zhong Ying,Wenjing Yang,Weiwei Lin,Xiangchun Meng,Chengxue Wang,Fengyu Zhao
An efficient green process was developed for production of p -aminophenol (PAP) from hydrogenation of nitrobenzene (NB) over a traditional Pt/Al 2 O 3 catalyst in a reaction medium of supercritical CO 2 (scCO 2 ) and H 2 O without any additional acid catalyst involved. The combination of scCO 2 and H 2 O was confirmed to be effective for the production of PAP. The acidity, aroused by the in situ formed carbonic acid, increased with CO 2 pressure, which acted as acid catalysis during the reaction, and it can easily self-neutralize by depressurization of CO 2 , resulting in a green and a intensive process for it removed the final neutralization and salts disposal of the traditional liquid acids. Under the optimal reaction conditions, a high yield to PAP (68.9%) was achieved at the high conversion of NB (98.5%). Moreover, the results of in situ diffuse reflectance FTIR spectra revealed that CO was generated by the reverse water-gas shift reaction (CO 2 + H 2 → CO + H 2 O), it can adsorbed on the surface of Pt/Al 2 O 3 to suppress the undesired deep hydrogenation of N -phenylhydroxylamine (PHA) to aniline (AN), which also contributed to the obtained high selectivity of PAP. Therefore, the present green and efficient catalysis process will arouse the interest of researchers in the fields of the green and sustainable organic synthesis.
研究领域:
绿色化学
·
有机合成
·
催化化学
·
环境友好工艺
·
工业化学
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DOI
高影响因子
Journal of CO2 Utilization
·
2022
·
IF 8.321
Ye Qu,Yanglin Chen,Yifei Ye,Ping Xu,Jianmin Sun
Heterogenization of homogeneous catalysts without the loss of activity is still a huge challenge. Herein, homogeneous [HTMG][His][I] amino acid ionic liquid (IL), consisting of 1,1,3,3-tetramethylguanidine cation, histidine anion and iodine anion, were introduced into the pore channels of SBA-15 substrate with the assistance of supercritical CO 2 (scCO 2 ) media. Due to its low viscosity, high diffusivity and absence of surface tension, scCO 2 enabled [HTMG][His][I] to highly disperse in SBA-15 pore channels. Surprisingly, [HTMG][His][I]/SBA-15 heterogeneous catalyst displayed higher CO 2 cycloaddition activity (95% propylene carbonate yield) than equivalent molar pristine [HTMG][His][I] homogeneous catalyst (69% propylene carbonate yield) under the identical conditions. The significantly enhanced activity was resulted from the synergistic effect of [HTMG][His][I] and SBA-15 support. Moreover, [HTMG][His][I]/SBA-15 performed outstanding universality of various epoxides and reusability. This work developed a promising strategy to heterogenization of homogeneous IL catalyst assisted by scCO 2 as synthetic media and provided an efficient catalyst for CO 2 conversion.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Yichen Jiang,Dazhi Li,Yifei Zhao,Jianmin Sun
Hydrogen bond donor functionalized poly(ionic liquids) were incorporated into MIL-101 framework for synthesis of composites PIL-R@MIL-101 (R = COOH, OH, NH 2 ). The effect of different hydrogen bond donors on CO 2 -epoxide cycloaddition reaction was discussed through XPS, NH 3 -TPD characterizations. Thereinto, PIL-COOH@MIL-101 showed efficient catalytic performance in the cycloaddition reaction of CO 2 and epichlorohydrin , 92.7% substrate conversion was obtained under 70 °C, 1.0 MPa, cocatalyst- and solvent-free conditions for 2.5 h. The improved activity was benefited from the synergistic effects of Lewis acidic Cr centers, carboxyl group, and nucleophilic Br - , together with the high surface area (1178 m 2 /g), and good CO 2 affinity. In addition, PIL-COOH@MIL-101 also showed facile recovery method by easy centrifugation and good recycling stability. Considering the good CO 2 affinity, excellent catalytic performance in CO 2 cycloaddition reaction, better thermal and recycling stabilities, the facilely prepared functionalized poly(ionic liquid)@MIL-101 composite would exhibit promising application prospect in CO 2 capture and conversion.
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PubMed
高影响因子
危险品化学品经营许可证（带存储）