FUEL
·
2020
·
IF 5.578
Limo He,Song Hu,Xiaofei Yin,Jun Xu,Hengda Han,Hanjian Li,Qiangqiang Ren,Sheng Su,Yi Wang,Jun Xiang
Fe-modified Ni/Al 2 O 3 catalysts with Fe/Ni molar ratios of 0, 0.5, 1 and 2 were prepared to promote the co-production of H 2 and carbon nanotubes (CNTs) during steam reforming of toluene as a tar model compound. After the addition of Fe, toluene conversion increased from 55.1% of Ni/Al 2 O 3 to 73.6% of F1N1A (Fe/Ni ratio of 1), and H 2 yield over F1N1A reached the maximum of more than 2000 mmol/(g-cata). Multi-walled carbon nanotubes with average diameter of 10–30 nm were generated and follow tip-growth mechanism. Compared with Ni/Al 2 O 3 , the addition of Fe remarkably increased the amount and quality of CNTs which had longer length and less tortuosity. These dual promoting effects on H 2 and CNTs after the addition of Fe were attributed to the strong interaction between Ni and Fe in Fe-Ni alloy. Fe-Ni alloy had the high activity for the decomposition performance of toluene and H 2 O to generate more H 2 and intermediates for improving the reforming reaction. Meanwhile, the high catalytic decomposition activity supplied more carbon species and the formation of Fe-Ni alloy enhanced the generation of metal carbide for promoting CNTs growth. Besides, the deposition of amorphous carbon was suppressed and the interaction between Ni particle and catalyst support was weakened after the addition of Fe, which kept the activity of catalyst and promoted the tip-growth of CNTs.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Lanhua Yi,Fujun Lan,Jinge Li,Caixian Zhao
Photocatalytic water splitting for H2 evolution is appealing for transforming solar energy into clean chemical fuel. This technique generally requires noble metals as H2 evolution cocatalysts to facilitate efficient cleavage of water. Herein, we report a noble-metal-free TiO2 nanobelts composite photocatalyst, in which TiO2 nanobelts are supported by nitrogen-doped graphene coordinated with a single Co atom (Co-NG). The results show that Co-NG is an efficient cocatalytst for the photocatalytic H2 production over TiO2. The optimal amount of Co-NG loading is found to be 3.5 wt %, showing a H2 evolution rate of 677.44 μmol h–1 g–1 under illumination of AM 1.5 G simulated sunlight, which is close to that of platinized TiO2 nanobelts and 2.6 and 31.2 times greater than that of 3.5 wt % NG/TiO2 nanobelts composite and pure TiO2 nanobelts, respectively. The significantly improved photocatalytic activity is ascribed to the remarkable synergistic effect between single-atom Co and N-doped graphene, which serve as effective H+ reduction sites and efficient electron acceptors, respectively. Besides, the Co-NG cocatalyst also effectively retards the recombination of photoinduced charge carriers and leads to a prolonged lifetime of charge pairs. This study reveals that Co-NG is an up-and-coming candidate as cocatalyst for development of cost-effective photocatalysts for efficient solar-driven H2 evolution.
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RSC Advances
·
2017
·Vol. 7
·期 46
·29184-29192
·
IF 3.108
Ting Song,Piyong Zhang,Jian Zeng,Tingting Wang,Atif Ali,Heping Zeng
C60/Fe2O3 nanocomposites are successfully prepared, well characterized, and employed in visible-light-driven photocatalytic H2 production. The Fe2O3 polymorphs show obvious broad-spectrum absorption, even close to the near infrared region (780–900 nm). The H2 production rates of β-Fe2O3 and γ-Fe2O3 are almost 2.1 times and 3.1 times higher than α-Fe2O3 (which itself is close to that of g-C3N4). This demonstrates that carefully controlling the polymorphs can tune the photocatalysts' H2 production properties. After modifying the Fe2O3 polymorphs with C60, the sample with 0.5 wt% C60/β-Fe2O3 has the optimum photocatalytic activity. This result indicates that the strength of the interaction and interfacial contact between C60 and Fe2O3 polymorphs plays an important role in the enhancement of photocatalytic activity, which can improve the transmission efficiency of photogenerated electrons via a conjugated three-dimensional π system. Fluorescein is introduced as a photosensitizer and the optimum mass ratio of fluorescein + 0.5C60/β-Fe2O3 is 1 : 1, which significantly boosts the photocatalytic H2 evolution rate of 0.5C60/β-Fe2O3 from 321.8 to 1665.0 μmol g−1 h−1. Meanwhile, the composites exhibit high stability and reusability.
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Nano Research
·
2017
·Vol. 11
·期 2
·1004-1017
·
IF 7.354
Wu Tianxing,Zhu Xiaoguang,Wang Guozhong,Zhang Yunxia,Zhang Haimin,Zhao Huijun
Electrocatalytic synthesis of value-added chemicals is attracting significant research attention owing to its mild reaction conditions, environmental benignity, and potentially scalable application to organic synthetic chemistry. Herein, we report the preparation of a single-crystalline NiS 2 nanostructure film of ∼ 50 nm thickness grown directly on a carbon fiber cloth (NiS 2 /CFC) by a facile vapor-phase hydrothermal (VPH) method. NiS 2 /CFC as an electrocatalyst exhibits activity for both the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER) in alkaline media. Furthermore, a series of alcohols (2-propanol, 2-butanol, 2-pentanol, and cyclohexanol) were electrocatalytically converted to the corresponding ketones with high selectivity, efficiency, and durability using the NiS 2 /CFC electrode in alkaline media. In the presence of 0.45 M alcohol, a remarkably decreased overpotential (∼ 150 mV, vs. RHE) at the NiS 2 /CFC anode compared with that for water oxidation to generate O 2 , i.e., the OER, in alkaline media leads to significantly improved H 2 generation. For instance, the H 2 generation rate in the presence of 0.45 M 2-propanol is almost 1.2-times of that obtained for pure water splitting, but in a system that employs an applied voltage at least 280 mV lower than that required for water splitting to achieve the same current density (20 mA·cm –2 ). Thus, our results demonstrate the applicability of our bifunctional non-precious-metal electrocatalyst for organic synthesis and simultaneous H 2 production.
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FUEL
·
2024
·
IF 6.7
Mengxue Ji,Jian Wen,Qiuyue Xu,Guanghui Wu,Pinghua Chen,Xibao Li,Hualin Jiang,Xubiao Luo
Environmental pollution and energy shortage are two major challenges facing humanity today. Photocatalytic technology, as a green and sustainable approach, is an important choice for effectively addressing these challenges. The formation of S-scheme heterojunctions and built-in electric fields can significantly improve the transfer and separation of photoinduced charge carriers, hence enhancing the efficiency of photocatalytic reactions, which is greatly significant for improving the performance of photocatalysts. In this study, a photocatalyst CdS/ZnIn 2 S 4 with a built-in electric field, which is an S-scheme heterojunction photocatalyst, was prepared by a simple solvothermal method. CdS/ZnIn 2 S 4 exhibited efficient visible-light-driven H 2 evolution from water, with a rate of 4.09 mmol g -1 h −1 , 3.60 and 2.80 times higher than that of CdS and ZnIn 2 S 4 , respectively, and an apparent quantum efficiency (AQE) of 2.71 %. Moreover, it also showed performance in visible-light-driven degradation of various ECs, achieving degradation rates of 82.2 %, 80.9 %, and 81.5 % for tetracycline, ciprofloxacin, and norfloxacin, respectively, within 40 min. It was confirmed that the successfully constructed S-scheme heterojunction can effectively separate photoinduced electron-hole pairs and suppress their recombination. The built-in electric field inside the composite material can effectively promote the movement of photoinduced charge carriers, thereby promoting the course of photocatalytic reactions. This study is positively significant for the development of novel efficient photocatalysts, exploration of new methods for environmental pollution control, and development of green hydrogen energy.
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高影响因子
ACTA PHYSICO-CHIMICA SINICA
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2025
·
IF 13.5
Yuge Fan,Xianliang Fu,Li Zhu,Man Xu
Low-temperature KSCN flux has been used for one-pot fabrication of decorated sulfide-based photocatalysts. However, the reaction system is actually short of S precursor, as it is determined by the decomposition of relatively stable KSCN, which may not be conducive to the production of high-performance catalysts. To this end, a modified KSCN flux route with a dosage of external S source was developed and used for the one-pot preparation of sulfide photocatalyst with 1% MoS 2 /CdS as the prototype. The results indicated that, compared with the sample (MC) prepared in conventional KSCN flux, a highly efficient sample enriched with seldom reported Cd vacancy (V Cd , MC-S) could be readily fabricated under the S 2− -rich environment. Furthermore, both the size of CdS and MoS 2 could be substantially reduced from μm to nm scale as more nuclei could be introduced in the flux, which leads to a few-layer MoS 2 that can be uniformly and tightly anchored on CdS with the average size of only ∼33 nm. Consequently, the resulting MC-S demonstrated an exceptional H 2 evolution activity of 15.01 mmol h −1 g −1 — a significant 6.5-fold improvement over its counterpart (MC) prepared through traditional KSCN flux. The high activity can be mainly ascribed to the introduction of V Cd and the close interface between small CdS and few-layer MoS 2 , which both benefit electron-hole separation. The preparation mechanism of the samples was tentatively compared and discussed from the difference in the nucleation and the development of crystals. We believe that this improved preparation method will also benefit the synthesis of other high-performance sulfide-based photocatalysts.
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高影响因子
Journal of Water Process Engineering
·
2024
·
IF 6.3
Jianan Dai,Chao Wu,Jing Ma,Shu-Hao Chang,Weiwei Liu
The conventional heterojunction formed by combining two different semiconductors is associated with issues of low compatibility, restricted intimate contact, and limited charge anti-recombination process. To address these issues, a simple strategy was adopted to fabricate a hetero-phase junction flanked with two dissimilar crystal phases of a single semiconducting material . This study employed TiB 2 as the initial material to fabricate an anatase/rutile TiO 2 hetero-phase junction material (AR-TiO 2 ), followed by its combination with highly conductive monolayer Ti 3 C 2 nanosheets to develop an AR-TiO 2 /Ti 3 C 2 composite photocatalyst . The photocatalyst displayed a wide range of light absorption and a remarkable capability for separating photogenerated carriers. The closely interconnected hetero-phase junction surface, formed by the rutile and anatase phases of AR-TiO 2 , combined with the incorporation of highly conductive Ti 3 C 2 nanosheets , synergistically increased the availability of multi-dimensional active sites and increased the efficacy of separating photogenerated electron pairs. The optimized AR-TiO 2 /Ti 3 C 2 achieved a degradation efficiency of 91.49 % for tetracycline hydrochloride (TCH) within 2 h and produced 1005.81 μmol of hydrogen in 6 h. The impacts of initial pH, co-existing anions, initial TCH concentration, initial temperature, and various pollutant species on the catalytic efficiency were also investigated. pH was shown to have the greatest impact on the photocatalytic performance of AR-TiO 2 /Ti 3 C 2 for TCH degradation. •O 2 − , and h + were identified as the primary reactive species that enabled the photocatalytic performance of AR-TiO 2 /Ti 3 C 2 through trapping experiments. This study presents a novel method to synthesize hetero-phase junction photocatalysts and suggests that Ti 3 C 2 has potential prospects for use in photocatalysis .
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2017
·
IF 9.446
Zhifeng Jiang,Kun Qian,Chengzhang Zhu,Hongli Sun,Weiming Wan,Jimin Xie,Huaming Li,Po Keung Wong,Shouqi Yuan
Photocatalytic H 2 evolution from water splitting requires an efficient photocatalyst with excellent charge separation ability and broad visible-light adsorption region. 0D CdS-TiO 2 nanodots (NDs) were successfully decorated on the 2D g-C 3 N 4 sheets via an epitaxial growth process. The as-synthesized ternary composite of CdS-TiO 2 @g-C 3 N 4 exhibits enhanced visible-light-driven photocatalytic H 2 evolution activity, as compared to the binary composites and their single components, which is about 6.7 and 11.2 times higher than those of single CdS and g-C 3 N 4 , respectively. Moreover, the as-obtained ternary composite has an external quantum efficiency (EQE) of 11.9% at 420 nm, implying the high utilization efficiency of photo-induced charges. In addition, the superior photostability can be achieved by this coupling method. The enhanced photocatalytic activity was attributed to the efficient charge separation originated from the three-level electron transfer system, the matched energy level positions, the abundant adsorption sites and active sites (0D/2D structure) and the synergistic effect among CdS, TiO 2 and g-C 3 N 4 . The work present here demonstrated that the construction of this three-level electron transfer system is an effective strategy to design more efficient ternary materials toward solar energy conversion (like H 2 production and CO 2 reduction).
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高影响因子
FUEL
·
2022
·
IF 8.035
Yuzhuo Wang,Yingjie Li,Liguo Yang,Xiaoxu Fan,Leizhe Chu
Co-gasification of biomass and waste plastics is a promising technology for H 2 production. In this work, Ni-CaO-Ca 12 Al 14 O 33 and Ni-CaO-MgO bi-functional materials were prepared from carbide slag for H 2 production in sorption-enhanced steam gasification experiments of cellulose/polyethylene mixtures. The H 2 production and CO 2 capture performances of Ni-CaO-Ca 12 Al 14 O 33 and Ni-CaO-MgO in sorption-enhanced steam gasification of cellulose/polyethylene were studied and compared. Density functional theory calculations, including the density of states, electron differential densities, and adsorption energies were performed to investigate the effect of supports on the stability and reactivity of Ni-CaO-based bifunctional materials at a microscopic level. The results exhibit that polyethene contributes to improving the H 2 production effectiveness of cellulose sorption-enhanced steam gasification, the optimum mass ratio of cellulose to polyethene is 0.5:0.5. The CO 2 capture capacity, H 2 yield, and H 2 concentration using Ni-CaO-Ca 12 Al 14 O 33 can be respectively 2.0, 2.6, and 1.4 times as high as those using Ni-CaO-MgO in the 20th cycle, which indicates the higher cyclic stability and catalytic activity of Ni-CaO-Ca 12 Al 14 O 33 . Density functional theory results also indicate that Ca 12 Al 14 O 33 can better retain the stable structure of Ni-CaO-based materials, which is consistent with the experimental results. Compared with MgO, Ca 12 Al 14 O 33 is a better framework for Ni-CaO-based bifunctional material for H 2 production in the sorption-enhanced steam gasification process.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Shuzhuang Sun,Bocheng Yu,Yu Liu,Bin Lu,Yanmei Shen,Yanmin Zhang,Hongman Sun,Hui Zhou,Hengshan Qiu
Integrated carbon capture and utilization via dry reforming of methane (ICCU-DRM) paves a sustainable way for directly converting CO 2 from flue gas into CO. However, the process suffers from severe carbon depositions and low CH 4 utilization. Herein, we demonstrate that the NiMnxCa dual functional materials undergo a spontaneous structural self-optimization during cyclic ICCU-DRM process. The MnO x can segregate from (MnO) α (CaO) 1-α solid solution during CO 2 capture. Consequently, the Ni-MnO x interaction, with a MnO x -coated Ni surface, can be intensified with the material reconstruction, which effectively suppresses the hydrogen recombination probability and prevent carbon deposition. Moreover, the *H from CH 4 activation can react with MnO, enabling highly efficient conversion of CO 2 via in situ chemical looping pathway. As an example, the NiMn5Ca achieved a ~ 100 % H utilization (~ 0 H 2 production), 95 % CO 2 conversion and < 1 carbon deposition/per mol of converted CO 2 at 675 °C in 25 cycles. The work illustrates a typical scenario of an intelligent structure optimization under reaction environment and proposes a strategy to enhance CH 4 utilization efficiency by directing *H to a fast surface reaction rather than desorbing as H 2 .
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高影响因子
GREEN CHEMISTRY
·
2025
·
IF 9.2
Xue Bai,Yanzhi Sun,Jiahong Xie,Huayi Yin,Rui He,Zhenfa Liu,Xifei Li,Junqing Pan
The sluggish leaching kinetics and low separation efficiency of Li/Co/Ni ions with high chemical consumption greatly hindered the recovery efficiency and cost of spent Li-ion batteries. Herein, we propose a self-generated H2 drives gradient reduction of spent cathode via surface enrichment of Li+ from retired Li-ion batteries, achieving a facile, efficient extraction of Li (>99.3%) by water as a leaching agent without chemicals. Characterizations and calculations reveal the adsorption and electron transfer mechanism between H2 and LiCoO2, the new phase transition mechanism of the layered structure and the changes in the electronic bonding and coordination environment of elemental Co during H2 precise reduction. Economic and environmental analyses showed that this work exhibits 22.6% energy consumption with 0% CO2 emissions and chemical consumption than hydrometallurgy, respectively, fully demonstrated its green and energy saving prospects for recycling spent Li-ion batteries.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2011
·
IF 4.749
Quan Gu,Xianliang Fu,Xuxu Wang,Shifu Chen,Dennis Y.C. Leung,Xiuqiang Xie
The adsorption behavior and the photocatalytic reforming (PR) process of 2-propanol over Pt (1 wt.%)/TiO 2 (PT) photocatalyst have been investigated by Fourier transform infrared (FTIR) spectroscopy. Both the adsorption complexes and the reforming intermediates formed on the PT and the gas-phase were determined and identified by FTIR spectra. The results indicated that the first layer surface of the PT mainly consisted of chemisorbed 2-propanol (Ti–OCH(CH 3 ) 2 ) through the condensation of 2-propanol with surface Ti–OH or dissociative adsorption with undercoordinated Ti atoms, while the second layer consisted of physisorbed 2-propanol by interaction with the chemisorbed one or the formed H 2 O via hydrogen-bond. Under UV irradiation, a rapidly deprotonation of 2-propoxide occurred by the attack of holes (h + ) and resulted in the formation of acetone, which was then slowly oxidized to acetate and formate species by the hydroxyl radicals ( OH). The carboxylates finally decarboxylate over the PT to evolve CO 2 and CH 4 via the photo-Kolbe reaction. According to the results, a reforming mechanism was proposed. The role of the OH groups contained in 2-propanol and its intermediates were found to serve as anchors for their adsorption and to involve the formation of h + transport ways.
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危险品化学品经营许可证（带存储）