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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高影响因子
Journal of CO2 Utilization
·
2017
·
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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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
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yongbiao Sun,Hui Li,Haijun Lai,Yan Yu,Meiling Hou,Chao Fu,Zaizhou Wang,Chunxiang Zhang
Natural gas purification before liquefaction necessitates the use of efficient adsorbents with high selective CO 2 adsorption and easy regeneration. Because of its efficiency and ease of operation, the ion exchange is widely employed to adjust zeolites’ CO 2 adsorption. However, few in-depth mechanistic studies have been undertaken on cation substitution regulation of pore structure and gas–solid interaction, as well as their synergistic effects on CO 2 selective adsorption and zeolite regeneration. In this study, we synthesized Li + and K + -modified 13X and examined their material characteristics, thermodynamics, adsorption kinetics, and the adsorption–desorption performance under various desorption methods. The results showed that the variation in pore structure and gas–solid interaction with cation radius is non-monotonic, resulting in 13XLi and 13XK having better CO 2 selective adsorption than 13X. All zeolites are extremely stable after 10 adsorption–desorption cycles in each regeneration setting. 13X outperforms 13XLi and 13XK in CO 2 desorption at 30 °C, owing to its large non-micropore volume and low gas–solid interaction. 13XK has the lowest CO 2 desorption rate at low temperature but the highest at high temperature, owing to the flat micropore distribution and the progressive gas–solid interaction. Approximately 100 % regeneration of 13XK is achieved with CH 4 purging (150 mL/min) at 150 °C, owing to its smallest cumulative pore volume at 0.5 nm. This research could help to develop efficient cation-modified X zeolites for CO 2 deep removal from CH 4 streams prior to liquefaction, as well as advance the in-depth understanding of cation substitution mechanisms.
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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
·
化学工程
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高影响因子
Science China-Chemistry
·
2020
·Vol. 63
·期 12
·1721-1726
·
IF 6.356
He Chaohua,Chen Sijia,Long Ran,Song Li,Xiong Yujie
The sharp rise of CO 2 in the atmosphere has become a potential threat to global climate, which results from the massive utilization of fossil fuel since the industry revolution. CO 2 electroreduction provides us a new possibility of utilizing CO 2 as a carbon feedstock for fuel and commercial chemicals generation. In this article, a new method is developed for synthesizing CuInS2 hollow nanostructures through the Kirkendall effect. The CuInS 2 hollow nanostructures exhibit excellent catalytic activity for electrochemical reduction of CO 2 with particular high selectivity, achieving high faradaic efficiency for HCOOH of 72.8% at −0.7 V. To elucidate the mechanisms, operando electrochemical Raman spectroscopy is employed to examine the CO2 reduction process. This work provides new insights into the design of hollow nanostructures toward electrocatalytic CO2 conversion and offers us an effective and reliable way for real-time investigation of electrochemical CO2 reduction reaction processes.
研究领域:
材料科学
·
电催化
·
环境科学
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高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 31
·15884-15890
·
IF 11.301
Rong Xia,Sheng Zhang,Xinbin Ma,Feng Jiao
Rational design and synthesis of efficient catalysts for electrochemical CO2 reduction is a critical step towards practical CO2 electrolyzer systems. In this work, we report a strategy to tune the catalytic property of a metallic Pd catalyst by coating its surface with a polydiallyldimethyl ammonium (PDDA) polymer layer. The resulting PDDA-functionalized Pd/C catalysts exhibit an enhanced CO faradaic efficiency of ∼93% together with a current density of 300 mA cm−2 at −0.65 V versus reversible hydrogen electrode in comparison to non-functionalized and commercial Pd/C catalysts. X-ray photoelectron spectroscopy analysis reveals that the improvement can be attributed to the electron transfer from the quaternary ammonium groups of PDDA to Pd nanoparticles, weakening the CO binding energy on Pd. The weak CO adsorption on Pd was further confirmed by the CO temperature programmed desorption measurement and operando attenuated total reflection-Fourier-transform infrared analysis. Therefore, the incorporation of electron-donating groups could be an effective strategy to decrease the CO binding energy of a metallic catalyst for a high CO selectivity in CO2 electroreduction.
研究领域:
化学
·
材料科学
·
环境科学
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高影响因子
Journal of the American Chemical Society
·
2026
·Vol. 148
·期 30
·32768-32781
·
IF 16.6
Feng Kai,Qian Shuairen,Liu Xiaozhi,Shen Yang,Li Zhengwen,Chen Yuxin,Tian Jiaming,He Le,Zhang Xiaohong,Cheng Yi,Su Dong,Yan Binhang
The Haber–Bosch ammonia synthesis is a cornerstone
of global
agriculture and the chemical industry, yet it is fundamentally constrained
by intrinsic scaling relations, necessitating energy-intensive conditions
associated with a significant carbon footprint. Herein, we report
a surface redox-mediated chemical looping strategy that utilizes the
CO 2 hydrogenation reaction as a chemical trigger to drive
ammonia synthesis at atmospheric pressure over a cobalt–molybdenum
bimetallic nitride (Co 3 Mo 3 N) nitrogen carrier.
Mechanistic investigations reveal that CO 2 induces a dynamic
surface oxidation that weakens the intrinsic Mo–N bonds and
facilitates the hydrogenation and release of lattice nitrogen as NH 3 . The cycle is closed by a subsequent nitridation step that
removes surface oxygen and regenerates the nitride lattice. This redox-mediated
mechanism enables an unprecedented NH 3 peak concentration
of ∼2.3% and a release rate of 12.4 mmol·g cat –1 ·h –1 at 500 ° C under
atmospheric pressure, circumventing the thermodynamic limitations
that historically hinder low-pressure ammonia synthesis. Our findings
demonstrate how dynamic surface engineering can decouple kinetic limitations
from thermodynamic constraints, offering a novel paradigm for sustainable
nitrogen fixation coupled with carbon utilization.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Jiaojiao Xie,Xinyu Zhi,Bowen Lu,Dikun Hong,Liqi Zhang
NiFe 2 O 4 has been widely applied in CO 2 hydrogenation for its excellent redox properties. However, NiFe 2 O 4 samples usually exhibited complex performance, rapid inactivation followed by slow activation, and poor hydrogenation selectivity. In this work, the complex behavior of NiFe 2 O 4 in CO 2 hydrogenation was studied, and the influence of surface oxide species(NiO and Fe 2 O 3 ) on its catalytic performance was probed on NiFe 2 O 4 -ww through magnetic water washing. NiFe 2 O 4 -ww was observed to predominantly produce CO with nearly 100% selectivity at lower temperatures and demonstrated a higher CO 2 conversion rate of 71.90% at 700 °C. However, under high-temperature reducing conditions, NiFe 2 O 4 -ww underwent rapid reduction to form Fe Ni alloy, which induced sintering and carbon deposition, thereby leading to a significant decline in catalytic activity. Surface NiO species on NiFe 2 O 4 enhanced CO 2 hydrogenation at lower temperatures but reduced the selectivity towards CO. Surface Fe 2 O 3 species enhanced the catalytic resistance to reduction, thereby improving catalyst stability by inhibiting the accumulation of carbon deposition. The effect of residual oxides on the NiFe 2 O 4 surface may give insight into understanding the deactivation behavior of Fe Ni alloy in CO 2 hydrogenation.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Chouqiang Li,Yunying Zhao,Guohui Li,Yu Deng
Carbon dioxide (CO₂) is a major greenhouse gas, with significant emissions from fossil fuel combustion and biological activities. CO₂ emissions from biological processes are particularly dispersed and variable, making capture and carbon utilization challenging. In this study, by coupling the engineered biosynthesis of polyamine with self-driven in situ CO₂ capture, we successfully achieved efficient CO₂ fixation. In particular, an acid-resistant cadaverine-producing lysine decarboxylase (CadA) was transformed using surface engineering to yield the effective alkali-resistant mutant CadA-M2, which exhibited the lowest K m and highest k cat /K m in the range of pH 7.0 to 10.0. Then 297.0 g/L of cadaverine was achieved in a 5 L single-batch bioreactor, the highest reported titer to date, while 85% of released CO₂ was converted to bicarbonate and utilized to synthesize C 3 compound malonic acid, yielding diamines and dicarboxylic acids of the two key nylon precursors. This integrated approach seamlessly combined cadaverine production with efficient CO₂ capture and conversion, providing a groundbreaking pathway for utilizing CO₂ from biological processes in sustainable chemical manufacturing and advanced carbon management technologies.
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高影响因子
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