INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2017
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IF 3.582
Zuohua Liu,Yujie Zheng,Tingting Gao,Jing Zhang,Xuefeng Sun,Guowei Zhou
In this study, anatase TiO 2 nanorods with exposed high-energy {100} and {001} facets and low-energy {101} facets were fabricated in the presence of surfactants cetyltrimethylammonium bromide , didecyldimethylammonium bromide, and ammonia via a facile hydrothermal method without the erosive reagent hydrofluoric acid . The particle size and morphology were mainly tuned by regulating the hydrothermal temperature. When the temperature was increased from 150 °C to 180 °C and 200 °C, the length of the nanorods decreased from 700-1000 nm to 400–500 nm and 100–200 nm, respectively. Concurrently, the edges and tops of the truncated tetragonal pyramid of the TiO 2 nanorods became blurry and flattened. The synthesized typical TiO 2 nanorods were then used as photocatalysts , and their performance during the direct generation of H 2 from water was evaluated. The TiO 2 nanorods obtained at 150 °C successfully produced high amounts of H 2 evolution (281.36 μmol) in the presence of methanol as a sacrificial agent under ultraviolet light irradiation for 4 h. The outstanding photocatalytic activity of the nanorods was mainly ascribed to the formation of surface heterojunctions in the edges and corners between adjacent high-energy {001} or {100} facets and low-energy {101} facets. The formed heterojunctions could facilitate charge separation through preferential carrier flow toward the specific facets.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Jiajin Li,Minglei Lu,Yuxin Ge,Weiwei Lu,Zidi Liu,Hongde Xu,Yu Zhang,Zhihui Li,Zhuoyu Zheng,Pengxiang Gao,Qian Zhang,Tiejun Wang
Aqueous-phase reforming of methanol (APRM) is an important method for H 2 production, widely used in energy fields like polymer electrolyte membrane fuel cells (PEMFCs). However, traditional noble metal catalysts , being expensive and vulnerable to CO poisoning, restrict their practical application. Therefore, developing robust non-noble metal catalysts for efficient and sustainable H 2 production with low CO levels in APRM at low temperatures is highly significant. In this study, a novel approach was employed to synthesize carbon-encapsulated Cu catalyst via controlled pyrolysis , leading to Cu@CA-Val catalyst with excellent low-temperature catalytic activity. The optimal Cu@CA-Val-300 catalyst exhibited a high hydrogen production rate of 0.2–27.0 μmolH 2 /g cat /s over a wide temperature of 135–180 °C (base-free), surpassing the most Cu-based and Pt-based catalysts. The Cu@CA-Val-300 catalyst exhibited exceptional hydrothermal stability during continuous operation in a fixed reactor for 200 h. Efficient H 2 production was attributed to good wettability , enabling the diffusion of CH 3 OH and H 2 O molecules into Cu + /Cu 0 sites for activation, with CO being suppressed and transformed through the formate formation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Chong Chen,Qiuhao Li,Fengqing Wang,Changjiang Hu,Jun Ma
Precise defect engineering of photocatalysts is highly demanding but remains a challenge. Here, we developed a facile and controllable γ-ray radiation strategy to assemble dual-vacancies confined MoS 2 -CdS-γ nanocomposite photocatalyst. We showed the solvated electron induced homogeneous growth of defects-rich CdS nanoparticles, while the symbiotic • OH radicals etched flower-like 1T/2H MoS 2 substrate surfaces. The optimal MoS 2 -CdS-γ exhibited a H 2 evolution rate of up to 37.80 mmol/h/g under visible light irradiation, which was 36.7 times higher than that of bare CdS-γ, and far superior to those synthesized by hydrothermal method. The microscopic characterizations and theoretical calculations revealed the formation of such unprecedented dual-sulfur-vacancies ensured the tight interfacial contact for fast charge separation. Besides, the existence of 1T-MoS 2 phase further improved the conductivity and strengthened the adsorption interaction with H + intermediate. Therefore, the radiolytic radical chemistry offered a facile, ambient and effective synthetic strategy to improve the catalytic performances of photocatalytic materials.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Honglin Yu,Peng Zhang,Mengqi Liu,Daiming Liu,Guodong Zhang,Fei Wang
Although clathrate hydrates were thought to open the Pandora box of hydrogen moderate storage, poor hydration efficiency of hydrogen hydrates impedes its application in hydrogen economy. To improve the situation, an efficient kinetic promoter of cetyltrimethylammonium bromide (CTAB) was proposed to enhance the hydration efficiency of mixed H 2 and 1,3-dioxolane (DIOX) hydrates, the micro structures of which were characterized via Raman spectra. In DIOX system, when CTAB was introduced, hydrate induction time reduces by 91.4 %, hydrate growth rate increases by 185.2 %, and the storage capacity of hydrogen in hydrates is up to 0.582 wt% under a moderate condition (12 MPa, 274.15 K), which increases by 99.32 %. Potential mechanisms behind the enhancement were proposed, and it was deduced that CTAB changes the arrangement of interfacial water molecules and induces hydration shells, which decrease the nucleation energy barrier as confirmed by the profiles of differential scanning calorimetry (DSC), giving rise to fast hydrate nucleation. In addition, hydrogen molecules were thought to enter the cavity of CTAB micelles, which serve as hydrogen vehicles to enhance the mass transfer of hydrogen by interfacial capture and inner release, resulting in fast hydrate formation. To the best of our knowledge, CTAB presents the best promotion effect on the nucleation and growth of H 2 /DIOX mixed hydrates among known kinetic promoters, and this finding promotes the application of clathrate hydrates on hydrogen moderate storage a small step forward.
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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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APPLIED SURFACE SCIENCE
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2024
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IF 6.3
Yu Huang,Xinyang Xu,Fengkun Han,Xi Chen,Guangjian Fan
Photocatalytic technology holds promising prospects for remediating naphthalene pollution in water bodies. In this work, the CN/Pt-P25 photocatalyst was successfully prepared via photodeposition combined with co-pyrolysis methods, and employed for naphthalene photodegradation under simulated sunlight. The chemical state of Pt was found to have a significant impact on the photocatalytic activity. H 2 secondary annealing effectively tuned Pt chemical states, increasing the proportion of Pt 0 species on the CN/Pt-P25 photocatalyst from 41.91 % to 62.24 %. The improved proportion of Pt 0 species proportion led to a reduction in the bandgap, which induced changes in the band positions and notably enhancing the separation efficiency of photogenerated electron-hole pairs. Under simulated sunlight irradiation, (H 2 ) CN/Pt-P25 photocatalyst achieved complete naphthalene photodegradation within 100 min. Thus, photocatalysts containing a high proportion of Pt 0 species exhibited an improved performance in naphthalene photodegradation. These findings provide new insights into the application of photocatalytic technology for the remediation of PAHs.
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ACS Sustainable Chemistry & Engineering
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2024
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IF 7.1
Yonghou Xiao,Qiang Guo,Shuohan Yang,Qidong Zhao,Gaohong He
The cuprous-ion-based zeolites constructed by introducing Cu(I) adsorption active sites into zeolite Linde Type A have proved to be efficient in carbon monoxide (CO) adsorption with high selectivity and capacity. However, how to directly fabricate zeolite 4A containing copper species and effectively overcome cuprous ion aggregation during the preparation process is still a challenge. Here, we propose an efficient fabrication method to synthesize highly dispersed Cu(I)-modified octahedral zeolite 4A adsorbents using a molecular complex formed by a hydrogel with a silicon/aluminum molar ratio of 1:1, copper ions, and tetramethylammonium hydroxide (TMAOH) as the template. Zeolite 4A containing copper ions was directly obtained by incorporating the precursor of cuprous ions into the confined space between zeolite 4A channel walls and TMAOH. The target zeolite Cu(I)/4A adsorbent with highly dispersed Cu(I) was constructed after introducing VCl3 as the reducing agent via the solid-state dispersion method during the process of removing the template. In comparison with pristine zeolite 4A, a bimodal microporous pore size distribution was observed in as-synthesized Cu(I)/4A. Cu(I)/4A exhibited an enhanced static (1.15 mmol/g) and dynamic (0.0016 mmol g−1) CO adsorption capacity, respectively, at 25 °C and 1 bar. Moreover, Cu(I)/4A displayed a lower H2 adsorption capacity under identical conditions. Through calculation using the ideal adsorption solution theoretical (IAST) equation, the CO selectivity from the CO/H2 mixture on Cu(I)/4A attained ca. 16.95. Therefore, Cu(I)/4A with highly dispersed Cu(I) was successfully fabricated, and its excellent CO adsorption selectivity and capacity enable it to be potentially applied for the actual deep separation of CO/H2.
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COMPOSITES PART B-ENGINEERING
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2024
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IF 12.7
Cong Liu,Hefeng Li,Jiabao Zhu,Xianhua Huan,Ke Xu,Hongbo Geng,Xiaodong Guo,Lei Ge,Xiaolong Jia,Xiaoping Yang,Hao Wang
The emerging graphene oxide membranes (GOm) showcase superiority in molecule barrier applications, yet their hydrogen (H 2 ) barrier performance is still less than ideal due to the insufficient control of GOm assembly architecture. Here, molecular patch engineering, in which amino rich polyethyleneimine (PEI) is controllably introduced into the GO system, is proposed to construct a highly aligned self-supporting PGO membrane (PGOm) for exceptional H 2 barrier performance. Based on the non-covalent and covalent interactions between GO nanosheets and PEI, the assembly behavior of GO nanosheets from the liquid phase to the solid phase is efficiently optimized in both extension and alignment synergistically, resulting in the superior alignments of PGOm with a Herman's orientation factor as high as 0.86. Owing to the excellent alignments, the hydrogen permeability (P H2 ) of PGOm is substantially reduced to a mere 2.28 cm 3 cm/(cm 2 ·s·Pa)·10 −15 even at a high temperature of 80 °C, representing a remarkable three-order-of-magnitude decrease compared to GOm. Additionally, at 25 °C, the P H2 of PGOm-enhanced epoxy sandwich composites is minimized to 1.2 cm 3 cm/(cm 2 ·s·Pa)·10 −15 , approximately 50 times lower than that of pure EP. This highlights the significant potential of PGOm in enhancing the gas tightness of composite pressure vessels.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Jiawei Hu,Jiaming Li,Zhongyi Pu,Wen Xiao,Huan Yu,Zhihao Zhang,Fang Yu,Chao Liu,Qinfang Zhang
Heterostructured visible-light-responsive photocatalysts represent a prospective approach to achieve efficient solar-to-chemical energy conversion. Herein, we propose a facile self-assembly technique to synthesize NiO nanoparticles/C 3 N 5 nanosheets (NOCN) heterojunctions for hydrogen (H 2 ) evolution catalysis and hydrogen peroxide (H 2 O 2 ) production under visible light. In this regard, the black NiO nanoparticles (NPs) were tightly anchored on the surface of C 3 N 5 nanosheets (CNNS) to construct S-scheme NOCN heterojunction, enabling efficient charge separation and high redox capability. Obtained results elucidated that the incorporated NiO NPs significantly promote light-harvesting efficiency and photo-to-thermal capacity over the NOCN composites. The enhanced photothermal effect facilitates the charge carrier transfer rate across the heterojunction and boosts the surface reaction kinetics. Accordingly, the photocatalytic performances of CNNS for H 2 release and H 2 O 2 production can be manipulated by introducing NiO NPs. The modified photocatalytic properties of NOCN composites are ascribed to the synergistic effects of all integrated components and the S-scheme heterojunction formation. Impressively, the high H 2 evolution photocatalysis efficiency of NOCN nano-catalysts in seawater certifies their potential environmental applicability. Among all, the 12-NOCN nano-catalyst exhibits a higher photocatalytic efficiency for H 2 release (112.2 μmol∙g −1 ∙h −1 ) and H 2 O 2 production (91.2 μmol∙L −1 ∙h −1 ). Besides, the 12-NOCN nano-catalyst reveals excellent recyclability and structural stability. Additionally, the possible mechanism for photothermal-assisted photocatalysis is proposed. This work affords a feasible pathway to design photothermal-assisted S-scheme heterojunctions for diverse photocatalytic applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Keting Feng,Kangqi Wu,Kai Li,Weijun Wang,Shihui Gao,Jun Fan,Tao Sun,Enzhou Liu
Localized surface plasmon resonance (LSPR) effect plays a crucial role in the field of solar energy utilization. In this work, we successfully prepared a Cu 2-x Se/ZnSe S-scheme heterojunction with a broad-spectrum response using the hot-injection and low-temperature water bath method. Importantly, we demonstrated that the photothermal effect induced by the LSPR of nonstoichiometric Cu 2-x Se can significantly improve the slow kinetics of water splitting, resulting in an apparent activation energy reduction from 50.1 to 28.7 kJ·mol −1 . This improvement is responsible for achieving the highest photocatalytic H 2 evolution rate of 63.6 mmol·g −1 ·h −1 over 2.7 % Cu 2-x Se/ZnSe under the wavelength ranged from 200 to 2500 nm, which is 3.4 and 5.6 times higher than that of ZnSe and Cu 2-x Se, respectively. Furthermore, the composite exhibits a remarkable H 2 production rate of 0.108 mmol·g −1 ·h −1 under near-infrared spectroscopy (800<λ<2500 nm), while ZnSe shows limited capability in H 2 releasing. Additionally, Cu 2-x Se/ZnSe demonstrates distinct photocurrent response when λ > 800 nm. The enhanced performance in H 2 evolution can be attributed to the synergistic effect of LSPR-induced light absorption and S-scheme heterojunction, which not only expands the light absorption range to the near-infrared region but also facilitates hot electron injection, charge carrier separation and transfer, leading to a faster surface reaction kinetics. This study provides an effective approach for designing a broad-spectrum light responsive non-precious metal-based photothermal-assisted photocatalytic system.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Renzhi Xiong,Fangde Liu,Xiao Xiao,Yanhe Xiao,Baochang Cheng,Shuijin Lei
The photocatalytic reduction of CO 2 over CdS faces significant challenges due to dominant hydrogen evolution competition and inefficient CO 2 activation. Herein, a magnetic cobalt-doping strategy is proposed that fundamentally restructures the surface reaction dynamics of CdS, effectively switching the photocatalytic pathway from H 2 evolution to CO 2 reduction. It is demonstrated that cobalt incorporation markedly suppresses charge recombination while increasing the population of photogenerated electrons available for CO 2 activation. Density functional theory calculations uncover two critical doping effects: an upshifted d-band center that optimizes CO 2 adsorption and activation energetics, and a substantially reduced energy barrier for the formation of rate-determining COOH* intermediate. Crucially, the introduced cobalt species induce pronounced spin polarization, which facilitates the separation of charge carriers. This spin effect can be further amplified under an external magnetic field to improve photocatalytic performance. The synergistic interplay of these effects endows Co-doped CdS with an exceptional CO production rate of 2322.8 μmol g −1 h −1 under visible light irradiation and magnetic field application – a 10.9-fold enhancement over pristine CdS. This work pioneers a novel paradigm that concurrently addressing thermodynamic (reaction pathway), kinetic (energy barrier), and electronic-spin (charge separation) factors, providing new design principles for breaking activity-selectivity trade-offs in photocatalytic CO 2 reduction systems.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Jiuli Chang,Lili Wang,Zhanqiang Hu,Songsong Zhi,Dapeng Wu,Kai Jiang,Zhiyong Gao
Selective ethylene glycol oxidation reaction (EGOR) to specific C2 species offers a promising approach to pair with cathodic hydrogen evolution reaction (HER) for electrochemical upcycling of waste polyethylene terephthalate (PET) plastic into high-value chemicals and H 2 . Efficient catalyst with tailored adsorptive interaction strength with intermediates is pivotal to fulfill such a scenario. Herein, a self-supported PdNi/NF electrode with deposition of PdNi hybrid onto nickel foam (NF) substrate was prepared by a gentle replacement reaction, which demonstrated high catalytic activity for EGOR toward glycolate with high faradaic efficiency (90 ± 2 %), decent yield (0.7 ± 0.01 mmol h −1 cm −2 ) and acceptable stability at a low applied potential of 0.8 V, which enabled electrosynthesis of glycolate via electrooxidation of PET hydrolysate. Meanwhile, a self-supported Cu, Co bimetallic phosphide onto NF substrate (CuCoP/NF) was prepared for HER catalysis, which featured a low overpotential of 117 mV at cathodic current density ( J ) of −100 mA cm −2 and decent durability. The further pairing of anodic EGOR and cathodic HER enabled electrolysis of PET hydrolysate to coproduce glycolate and H 2 at an energy-saving manner. This work provides a viable paradigm for coproduction of glycolate and H 2 from electrochemical upcycling of PET plastic, and presents essential instruction for reclamation of obsolete resource via sustainable and waste-to-treasure manner.
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