THERMOCHIMICA ACTA
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2024
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IF 3.1
Guolan Dou,Liying Zhang,Deming Wang,Xiaoxing Zhong,Botao Qin
The study examined the oxidative pyrolysis of raw and residual coals extracted with tetrahydrofuran, as well as the CO/CO 2 /H 2 /CH 4 emissions at high temperatures (200∼900 °C). Tetrahydrofuran was found to extract aromatic and aliphatic hydrocarbons from lower metamorphic coal, as well as hydroxyl, increasing the specific surface area of char formed by oxidative pyrolysis of residual coal. The CO 2 /CO ratio was temperature dependent, and the increase period was fit by a polynomial and a linear function, with critical temperature of around 570 °C. The greater CO 2 /CO ratio of raw coal suggested that oxidative pyrolysis produced more CO 2 . The kinetic analysis showed that the change in activation energy is inconsistent with the gas production, and the gases were found to be proportionate to the specific surface area of the coal chars, implying that the char structure has a significant influence on gaseous product emissions and the coal oxidative pyrolysis at high temperatures is a diffusion-controlled heterogeneous reaction. The findings of this study could be useful for determining the status of coal fire.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2025
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IF 14.3
Wenjiao Chang,Honghuo Wang,Tingting Wu,Shuting Zhang,Yifan Li,Junying Wang,Yongqiang Yang,Lei Wang
Photocatalytic CO 2 reduction reaction is regarded as a potential strategy to convert greenhouse gases into valuable chemicals. However, achieving photocatalysts with high efficiency and target product selectivity under visible light still faces great challenges. Herein, sub-2 nm RuO 2 @TiO 2 (RTO) nanorods with lattice matching interface are rationally designed and prepared via a hydrothermal reaction step-by-step. Due to the strong interaction of the lattice-matched interface with the Ru-O-Ti bond, new energy levels have emerged at the interface, leading to effective visible light absorbance. Moreover, the photo-generated electrons could be transferred to the RuO 2 efficiently via the lattice-matched interface. As a result, the RTO photocatalyst exhibits superior CO 2 -to-CH 4 conversion performance of 15.6 µmol g −1 with a selectivity of 87.9% under visible light irradiation. Density functional theory (DFT) calculation reveals that the energy barrier of CO* to CO is significantly higher than that of *CHO, resulting in the preferential production of CH 4 . This work provides an effective strategy for designing photocatalyst with promoted visible light absorption and improved product selectivity.
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ACS Applied Materials & Interfaces
·
2024
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IF 8.3
Yuntao Qi,Bin Zhang,Dengrong Xue,Hui Zhang,Xiaoning Liu,Zhi Liu,Shichao Zhao,Zhuo Li,Fanchun Meng,Yong Qin
The catalytic conversion of CO2 to CO through hydrogenation has emerged as a promising strategy for CO2 utilization, given that CO serves as a valuable C1 platform compound for synthesizing liquid fuels and chemicals. However, the predominant formation of CH4 via deep hydrogenation over Ru-based catalysts poses challenges in achieving selective CO production. High reaction temperatures often lead to catalyst deactivation and changes in selectivity due to dynamic metal evolution or agglomeration, even with a classic strong metal–support interaction. Herein, we have developed a FeOx/Ru/Rutile multilayer epitaxial structure by depositing a FeOx layer onto the epitaxially grown RuO2 nanolayers on the surface of rutile nanoparticles. This multilayer epitaxial structure transformed into a structure in which Ru nanoparticles were decorated with FeOx layers with ultrastable strong metal-support interaction (SMSI). Subsequently, the FeOx decoration on Ru nanoparticles effectively shifted the dominant product from CH4 to 95% CO during CO2 hydrogenation. Remarkably, this catalyst exhibits exceptional stability and can be operated stably at 550 °C for a long time without apparent deactivation. Compared with the dynamic changes observed in supported Ru nanoparticles, the interaction between Ru and FeOx maintains their electronic states at different reaction temperatures. Furthermore, this Ru–FeOx interaction inhibits H2 activation capability, CO adsorption, and subsequent hydrogenation of CO. The transformation strategy employed here, which utilizes initial multilayer epitaxial structures, can be applied to construct SMSI to enhance metal catalysts’ catalytic performance.
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CHINESE JOURNAL OF CATALYSIS
·
2024
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IF 15.7
Yanru Zhu,Zhijun Zhang,Jian Zhang,Shuangjiang Jiang,Zhe An,Hongyan Song,Xin Shu,Wei Xi,Lirong Zheng,Jing He
ABSTRACT Photosynthesis is a potential strategy to enable endergonic process that usually needs high-temperature in thermochemistry to supply the energy for inert-bond activation and/or strong endothermic reaction . The conversion of CO 2 into value-added C 2 -oxygenates is a promising process to realize artificial photosynthesis , but suffers from relatively lower efficiency due to complex multi-electron (≥ 10) transfer processes and sluggish kinetics of C–C coupling. This work proposes an all-new H 2 O-promoted strategy for efficient production of C 2 oxygenates from the concurrent activation and subsequent co-conversion of CO 2 with CH 4 under photo-thermal cooperation, in which photocatalytic H 2 O-splitting derived active hydrogen species for CO 2 activation, and concomitant active oxygen species for CH 4 activation. A formation rate of as high as 2.05 mmol g −1 h −1 for C 2 -oxygenates (CH 3 CHO and CH 3 CH 2 OH) in a selectivity of > 86% has been afforded over SrTiO x supported CuCo under 200 °C and ultraviolet-visible illumination. It has been revealed that SrTiO x drives photocatalytic H 2 O-splitting under the excitation primary from ultraviolet light, paired Cu I /Cu 0 sites promote the formation of *CH x O intermediate from CO 2 , Co sites conduct CH 4 -to-*CH 3 , and C–C coupling of *CH x O and *CH 3 on adjacent Cu-Co facilitates the generation of C 2 -oxygenates.
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ACS Sustainable Chemistry & Engineering
·
2024
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IF 7.1
Xupeng Zhang,Kaiqian Li,Longxin Guo,Zhiping Xu,Shuduan Deng,Ying Liu,Gang Zhu
To effectively mitigate the global warming problem caused by excessive CO2 emissions, the implementation of direct air capture (DAC) technology has emerged as one of the most promising strategies for capturing CO2 from the atmosphere. The key to DAC technology hinges on the development of high-performance solid sorbent materials that demonstrate high CO2 adsorption capacity and gas separation selectivity, particularly under low CO2 partial pressure conditions. Herein, we have successfully developed a class of MOF@carboxylated wood sponge (MOF@CWS) hybrid sorbents, capable of efficient CO2 capture from low-concentration (less than 10,000 ppm) CO2 sources, achieved by embedding the porous MOF into carboxylated wood sponges (CWS) substrate via an in situ growth route. Within the MOF@CWS series, the CO2 uptake capacity of Mg-MOF-74@CWS is 3.61 and 2.65 mmol/g at 1 bar, 273 and 298 K, respectively, significantly higher than those of CWS and HKUST-1@CWS. Moreover, this material exhibited outstanding DAC performance, with the CO2 sorption capacity at 273 K up to 0.56 mmol/g from ambient air (ca. 400 ppm of CO2), surpassing most other solid sorbents. The obtained Mg-MOF-74@CWS also demonstrated exceptional CO2/CH4 separation performance, primarily due to the unique pore structure and augmented interaction between the CO2 molecules and the hybrid sorbents. The results of this study indicate that Mg-MOF-74@CWS has potential as an efficient solid sorbent for the DAC of CO2.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Tingting Ren,Yanqing Zhang,Suning Fu,Yuanming Hou,Jiaxin Wang,Jingyi Qin,Zhengzheng Xie,Jianjun Yang,Zhongjie Guan,Shilong Jiao,Qiuye Li,Xianwei Fu
Exploring well-designed photocatalysts with high-quality interfaces for converting CO 2 into value-added chemical fuels faces a great challenge. Herein, a 2D/0D S-scheme heterojunction of Cs 3 Bi 2 Br 9 nanosheet/BiOBr nanocrystal (CBB/BOB) photocatalysts is designed and synthesized by an in-situ growth strategy for photocatalytic CO 2 reduction. The S-scheme heterojunctions with atomic-level intimate interfaces greatly accelerate the separation and transfer efficiency of photoinduced carriers and improve the reduction ability of photogenerated electrons resulting in prominent photocatalytic activity toward CO 2 photoreduction. Consequently, the environment-friendly hybrids show impressive photocatalytic CO 2 reduction efficiency and high CH 4 selectivity with a CH 4 yield and selectivity of 12.8 μmol g −1 h −1 and 79 %, respectively, which is 43 and 2 times higher than that of pristine CBB, respectively. The detailed experimental characterization and theoretical calculations indicate that the high adsorption/activation capability of CO 2 molecules and CO* intermediates and the lowered free energy of CO 2 reduction promote the photoconversion of CO 2 to CH 4 on the CBB/BOB heterojunctions. This work provides a new strategy for constructing perovskite-based photocatalysts for solar fuel applications.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Wanting Li,Ziqiong Wang,Jingli Zhai,Ling Zhang,Ruifeng Chong,Yanmei Zhou,Caixia Feng,Yan Wang
Photocatalytic CO 2 -to-CH 4 conversion via solar energy offers a sustainable carbon cycle pathway, yet its efficiency and selectivity are limited by the kinetically challenging eight-electron process. Herein, a sulfur vacancy-enriched NiS microflower hybrid decorated with carbon quantum dots (CQDs-X/NiS V ) is synthesized via hydrothermal method. Sulfur vacancies, induced in situ by NH₃ from thermal decomposition of NH 4 Cl and thiourea, serve as electron traps to promote carrier separation. The highly conductive CQDs facilitate rapid charge transport and enhance the CO 2 -to-CH 4 eight-electron reduction. A Schottky junction at the CQDs/NiS V interface further accelerates electron transfer from NiS V to CQDs, synergistically boosting CO₂ reduction. Experimental results reveal a positive correlation between CQD loading and sulfur vacancy concentration, elevating CH 4 yield from 0.19 to 2.47 mmol·g −1 . The optimal CQDs-100/NiS V achieves 2.47 mmol·g −1 CH 4 with 95.6 % selectivity. Notably, in diluted CO 2 atmosphere, the yield and the selectivity of CH 4 is apparently higher than that of in pure CO 2 due to the competition for photogenerated electrons between two reaction pathways: (1) CO 2 + 2e⁻ → *CO (2) *CO + 6e⁻ → CH 4 . This work provides a novel strategy for in situ generation of sulfur vacancies and a triple-strategy design (Schottky junction, CQD modification, defect engineering) for high-efficiency photocatalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Ziyi Li,Jia Xiong,Yufei Huang,Yangqiang Huang,Geoffrey I.N. Waterhouse,Ziyun Wang,Yu Mao,Zhiwu Liang,Xiao Luo
Photocatalytic CO 2 reduction reaction (CO 2 RR) is usually constrained by sluggish kinetics and low product selectivity. Herein, a Cu-doping multi-tier hierarchical S-scheme heterostructure Cu-ZnIn 2 S 4 /ZIF-67 was fabricated, achieving highly efficient photocatalytic CO 2 RR under visible light without additional thermal input. At low pressure (absolute pressure 40 kPa), the optimized catalyst 2Cu-ZISF demonstrated a CH 4 yield of 22.27 μmol g −1 h −1 with a selectivity of 94.7 %. In situ XPS and EPR confirmed that the photogenerated charge transfer obeys an S-scheme mechanism, with Cu sites serving as electron-rich centers, facilitating spatial charge separation. In situ DRIFT detected reaction intermediates of photocatalytic CO 2 RR mechanism, and Gibbs free energy calculations via Density Functional Theory revealed that Cu incorporation significantly stabilizes surface CO* species, thus reducing CO(g) production and facilitating hydrogenation, thereby acting as targeted active sites for CH 4 production. This work overcomes the limitations of slow reaction kinetics and offers an in-depth understanding of how to design effective S-scheme heterojunction photocatalysts and their charge transfer mechanisms.
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Nanomaterials
·
2025
·Vol. 15
·期 18
·1443
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IF 4.3
Shicheng Liu,Na Li,Qulan Zhou
Elucidating the mechanisms of CO2photocatalytic conversion systems is crucial for tackling the challenges of carbon neutrality. In this study, a series of Ag@g-C3N4photocatalysts were constructed with metal particle size modulation as the core strategy to systematically reveal the modulation mechanism of Ag nanoparticles (Ag NPs) size variation on the selectivity of CO2photoreduction products. Systematic characterizations revealed that increasing Ag size enhanced visible light absorption, promoted charge separation, and improved CH4selectivity. Photocatalytic tests showed Ag3.0%@CN achieved optimal activity and electron utilization. Energy band analyses indicated that Ag modification preserved favorable conduction band positions while increasing donor capacity. Further density-functional theory (DFT) calculations reveal that Ag NPs size variations significantly affect the adsorption stability and conversion energy barriers of intermediates such as *COOH, CO and CHO, with small-sized Ag7NPs favoring the CO pathway, while large-sized Ag NPs stabilize the key intermediates and drive the reaction towards the CH4pathway evolution. The experimental and theoretical results corroborate each other and clarify the dominant role of Ag NPs size in regulating the reaction path between CO and CH4. This study provides mechanistic guidance for the selective regulation of the multi-electron reduction pathway, which is of great significance for the construction of efficient and highly selective CO2photocatalytic systems.
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CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Haiyan Lu,Hu Zang,Changjiang Liu,Xin Liu,Wenli Xu,Nan Yu,Baoyou Geng
Copper-based catalysts exhibit moderate adsorption energy for *CO intermediates and have attracted significant attention for CO 2 electroreduction to fuels and high-value chemicals, but their low activity and poor selectivity remain challenges. Herein, we synthesized phosphorus-doped copper oxide (CuO x P y ) and demonstrated that phosphorus governs the phase transition, creating distinct interfaces that regulate proton donors or local OH – concentrations, thereby modulating the reaction pathway and directing CO 2 electroreduction selectively towards CH 4 or multi-carbon (C 2+ ) products. Notably, the P-Cu 2 O/Cu interface derived from amorphous CuO x P y exhibits a Faradaic efficiency (FE) for CH 4 of 53 % ± 4.99 % at a current density of 0.4 A cm −2 . In contrast, the Cu 2 P 2 O 7 /Cu 2 O interface obtained from crystalline CuO x P y achieves a FE C2+ of 74.3 % ± 1.75 % at 0.8 A cm −2 . Experiments and theoretical calculations reveal that the accumulation of proton donors at the P-Cu 2 O/Cu interface facilitates the protonation of the *CO intermediate, thereby enhancing CH 4 production. The Lewis acid sites of Cu 2+ at the Cu 2 P 2 O 7 /Cu 2 O interface enhance the local OH – concentration and lower the energy barrier for C-C coupling, resulting in high selectivity towards C 2+ products. This study presents a novel paradigm for the rational regulation of selectivity in CO 2 electroreduction products through modulation of the interfacial microenvironment.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Jialu Wei,Fanghui Mi,Wei Zhang,Chunwen Sun
BaCeO 3 -based proton conductors exhibit high ionic conductivity but suffer from poor chemical stability and high sintering temperatures, limiting their application in protonic ceramic fuel cells (PCFCs). This study demonstrates that Zn doping in BaZr 0.1 Ce 0.7 Y 0.2 O 3−δ (BZCY) enhances both chemical stability and ionic conductivity. BaZr 0.1 Ce 0.7 Y 0.1 Zn 0.1 O 3−δ (BZCYZn) achieves higher proton conductivities of 0.022 S cm −1 in humid H 2 and 0.019 S cm −1 in CH 4 at 750 °C, surpassing those of BZCY. Zn doping improves conductivity in both the bulk and grain boundaries. An anode-supported single cell using BZCYZn as the electrolyte delivers peak power densities of 1324.63 mW cm −2 in H 2 and 647.49 mW cm −2 in CH 4 , significantly outperforming BZCY. The electrochemical performance and mass transport properties of BZCYZn are further analyzed using distribution of relaxation times (DRT) analysis.
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APPLIED CATALYSIS A-GENERAL
·
2023
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IF 5.5
Shanhai Zhao,Chunhe Li,Kuankuan Ren,Zebo Fang,Ping Fang,Yanyan Zhu,Pengfei Fang
Photothermal catalytic CO 2 reduction is an attractive way to alleviate the current energy crisis, but it is important to prepare catalysts with efficient catalytic capacity. In this work, Prussian blue analogs were firstly prepared, and then calcined to obtain porous transition metal (Ni, Co, Fe) oxides (TMOs). The metal composition of catalysts has great influences on their structures and catalytic properties. Among them, NCF-TMO catalyst shows excellent photothermal catalytic performance, and can produce 2.9 mmol g -1 h -1 CO and 1.6 mmol g -1 h -1 mmol CH 4 at low CO 2 and H 2 concentrations. For the NCF-TMO, its superior catalytic performance mainly benefitted from two reasons: (1) The construction of heterojunction between NiO, Co 3 O 4 and Fe 2 O 3 , which promotes the efficient dynamic processes of charge carriers; (2) The formation of abundant surface reactive active sites facilitates the efficient conversion of CO 2 molecules. This study offers a bright direction for the resource utilization of CO 2 .
研究领域:
材料科学
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环境科学
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催化化学
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