Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Yuyan Wang,Hongxia Zhang,Wei Gao,Ming Zhong,Bitao Su,Ziqiang Lei
In this work, two series of plasmonic S-type heterojunction photocatalysts containing Bi, TiO 2 , and biochar (Bi/TiO 2 @C) have been developed through a biomass-assisted hydrothermal-calcination strategy, utilizing grapefruit peel as a reducing agent and C resource. The calcination temperature and the mass ratio of biomass were optimized to obtain the optimal nanocomposite, which shows excellent adsorptive and visible-light photocatalytic performance in the removal of diverse antibiotic and dye pollutants, including tetracycline, oxytetracycline, ciprofloxacin, sulfamethoxazole, sulfisoxazole, malachite green, and rhodamine B. The remarkable performance can be attributed to the enhanced absorption of light absorption resulting from the localized surface plasmon resonance effect of the semimetal Bi, and the formation of heterogeneous interface between Bi and TiO 2 , which accelerates the transfer of photogenerated charge. Furthermore, trapping tests and electron spin resonance (ESR) analysis reveal that ∙O 2 - and h + are the primary active species involved in the removal of tetracycline. A plausible charge transfer mechanism has been proposed.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Yang Wang,Dong Xu,Xuan Yang,Jing-Hui He
Organic pollutants, such as ciprofloxacin (CIP), are ubiquitously detected in wastewater. However, their removal remains a challenge for conventional wastewater treatment technologies. Photocatalysis and peroxymonosulfate activation coupling are considered a promising strategy for the removal of recalcitrant organic pollutants. However, identifying optimal photocatalysts that can effectively couple with peroxymonosulfate activation and induce synergistic degradation of organic pollutants remains a challenge to be addressed. In this work, a novel S-scheme inorganic–organic heterojunction BiVO 4 /Cu-TCPP (BC) was fabricated. In situ X-ray photoelectron spectrum showed that the strong internal electric field of the S-scheme heterojunctions enabled efficient carrier transport. The generated photogenerated electrons could activate the peroxymonosulfate, which further promoted the separation of the carriers. The BC-vis-peroxymonosulfate system achieved 93.1% ciprofloxacin removal in 10 min with apparent rate constants k of 0.2426 min −1 , which is larger than most reported peroxymonosulfate systems. Electron paramagnetic resonance spectra and liquid chromatography mass spectrometry demonstrated that the synergistic coupling of S-scheme heterojunction with peroxymonosulfate activation significantly improved the catalytic activity of the reaction system and enabled rapid CIP removal via both radical and nonradical pathways. The BC-vis-peroxymonosulfate system demonstrated ultra-fast removal of other quinolone antibiotics and organic pollutants and strong environmental adaptability under various conditions, suggesting its great potential for practical application. This study provides new insights for the design of efficient S-scheme heterojunction coupled peroxymonosulfate activation for environmental remediation.
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Journal of Energy Chemistry
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2025
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IF 14.9
Chenggong Niu,Yi Liu,Shuqing Zhou,Heyang Liu,Linyu Chen,Jingya Guo,Tayirjan Taylor Isimjan,Xiulin Yang
Triggering structural asymmetry can induce charge redistribution and modify electronic structures, which is of great significance for the design of high-performance hydrogen oxidation reaction (HOR) electrocatalysts. Herein, we propose a dual anion-induced strategy to create an innovative RuS 2 -RuO 2 heterostructure featuring abundant S-Ru-O interfaces (RuS 2 -RuO 2 @C). This RuS 2 -RuO 2 @C demonstrates an impressive mass activity of 2.61 mA μ g R u - 1 and an exchange current density of 2.96 mA cm −2 , surpassing Pt/C and other comparative samples by over 20 times. Durability assessments confirm the superior stability of RuS 2 -RuO 2 @C, with only minimal performance loss during operation. Density functional theory (DFT) calculations indicate that the asymmetric S-Ru-O configuration optimizes the interfacial electronic structure and shifts the d -band center closer to the Fermi level, effectively reducing the energy barrier of the rate-determining step (RDS) in the alkaline HOR process. Moreover, in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) characteristics disclose the formation of a substantial hydrogen bond network at the S-Ru-O interface, which aids in the desorption of H 2 O ad and facilitates the vital Volmer step in the HOR pathway.
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Science China-Chemistry
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2025
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IF 9.7
Liu Jie,Ye Qiu,Wu Yi,Chen Junliang,Ge Yongjie,Zhang Linjie,Abazari Reza,Qian Jinjie
Molecular catalysts like metal phthalocyanines (MPc) hold significant promise for diverse applications in renewable energy conversion and storage. Despite their inherent catalytic activity in the oxygen reduction reaction (ORR), enhancing their practical applicability necessitates addressing challenges in electrical conductivity and catalytic stability through effective control of electron distribution within the substrate. In this work, we have successfully synthesized an electrocatalyst featuring FePc molecules anchored onto N,S co-doped carbon nanorods from a pillar-layer metal-organic framework (MOF), designated as ZTB-NSCR-FePc. This MOF-derived heteroatom-doped carbon substrate could be easily obtained by direct pyrolysis of a pre-fabricated rod-like Zn-TDC-bpy. The optimized ZTB-NSCR-FePc demonstrated exceptional electrocatalytic efficiency and stability towards ORR with a positive half-wave potential of 0.890 V. When employed in a Zn-air battery, it outperformed the benchmark Pt/C air cathode, achieving a peak power density of 198.9 mW cm −2 . Finally, theoretical calculations revealed that short-range electron interactions between N/S atoms and the graphene substrate significantly enhance the anchoring effect of FePc, improve the adsorption of reaction intermediates, and thereby boost the ORR performance.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Renhui Ling,Mingxing Li,Xin Li,Laihuan Pei,Xiaoyan Luo,Congmin Wang
MOFs have high adsorption performance of ammonia (NH 3 ) because of its porosity and abundant coordination sites, especially MOFs containing carboxylic acid ligands have emerged as effect NH 3 adsorbents. But, it’s troublous for reversible ammonia adsorption for the strong metal-NH 3 coordination or the collapse of adsorbents. [MEDTA] 2- is a very stable and classic carboxylic acid-containing complex, but there was no relevant report. Therefore, this work carried out the design and synthesis of PVIm-R8-MEDTA based on the use of the coordination structure of [MEDTA] 2- and the stability of PILs’ skeleton. The characterization indicated the [MEDTA] 2- could be introduced into PILs successfully for the hydrogen bonding interactions with the imidazolium cation, and the obtained PVIm-R8-MEDTA presented enhanced NH 3 capacity (10.4–14.7 mmol/g) than their precursor PVIm-R8-Br (7.8 mmol/g). The mechanism of NH 3 adsorption was proposed by DFT calculation, spectroscopic method, and the calorimetric test, it indicated the NH 3 was fixed by imdazolium cation through hydrogen bonding and inserted into two of the carboxylate and metal bonds of [MEDTA] 2- . Because of the multi-meshing coordination of [EDTA] 4- and metal ions, the disconnected carboxylate ions could easily coordinate with metal ions again and repair the chelating structure of [MEDTA] 2- , which caused the ammonia easily be desorbed. In the process of gas adsorption, there was no bonding breakage of the skeleton of PILs, which helped the PVIm-R8-MEDTA be recovered under moisture and NH 3 atmosphere. Thanks for the designability of PILs, such as the cationic structure, structure and size of cross-linking agent, the choice of complex anion and so on, it provides a new design idea and theoretical basis for efficient and reversible ammonia adsorption materials.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Hao Jiang,Mei Yan,Hao Chen,Xue Chen,Yutuo Fu,Chongshen Guo
How to make full use of solar energy and improve the efficiency of charges separation of photocatalysis has been a concern for scientists all along. To achieve this, this work designed an n-n + homojunction of S-doped SnFe 2 O 4 and applied it to near infrared driven photocatalytic degradation and sterilization. The experimental results demonstrated that S doping significantly enhanced the photocatalytic performance of SnFe 2 O 4 . The degradation rate of ciprofloxacin and the removal rate of Staphylococcus aureus ( S. aureus ) reached up to approximately 65 % and 100 % after 6 h irradiation, respectively. The S-doping could increase the content of shallow trap states in SnFe 2 O 4 , effectively inhibiting the recombination of photogenerated electrons and holes. Moreover, S-doping also enhances the n-type character and forms n-n + homojunction. This n-n + homojunction generates a built-in electric field within the sample, which causes band bending and promotes photogenerated charges transfer and separation. Consequently, more carries are available for the generation of reactive oxygen species. Free radical quenching experiments and ESR tests show that •O 2 − is the main free radical in the photocatalysis. In addition, DFT calculations confirmed the enhanced activation of O 2 after S doping. This work provides a feasible way to effectively promote charges separation and transfer in metalloid-based photocatalysts.
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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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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Zhiyuan Ning,Xiangqian Tan,Qian Wei,Yue Liu,Ruigang Wang,He Guo,Jingyu Ren,Qiuling Ma,Jian Zhou,Tiecheng Wang
A nanoconfinement strategy was employed to encapsulate iron species within carbon nanotubes (Fe-CCNTs) in this study, enabling rapid degradation of sulfadiazine (SDZ) through sulfite (S(IV)) activation. The Fe-CCNTs catalyst enhanced the generation of reactive species during the S(IV) activation process. Nearly complete SDZ degradation was achieved within 10 min, with a reaction rate constant 1.8 times higher than that of the non-confined system. Fe-CCNTs shifted the mechanism from a radical pathway (SO 4 • − and •OH) to a non-radical pathway ( 1 O 2 and Fe IV =O), thereby improving SDZ degradation efficiency. The nanoconfinement effect increased the local charge density, accelerating electron transfer and promoting the formation of reactive species. This system exhibited strong catalytic performance, high reusability, and resistance to interference. Furthermore, the Fe-CCNTs/S(IV) treatment reduced the abundance of intestinal pathogenic bacteria and the toxicity of byproducts. The Fe-CCNTs/S(IV) system offers a promising and low-toxicity solution for antibiotic removal in water treatment.
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APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Wei Huang,Haojie Chen,Hefan Zhang,Xueying Wang,Chunlan Xu,Jiahao Liu,Lan Zhang,Changyu Lu
The design of green and low-cost S-scheme heterojunctions with strong interface interactions is key to their photocatalytic performance and practical application. Here, novel S-scheme heterojunctions of self-grown CuO/sediment (CUS) were successfully fabricated using a calcination method with sediment derived from nature. Various methods were employed to evaluate the micromorphology, crystal structure, chemical composition, and optical characteristics of the photocatalysts. Supported by ultra-violet photoelectron spectroscopy (UPS) analyses, an S-scheme charge migration path was revealed in the CUS during the photocatalytic reaction. The CUS3:7 S-scheme heterojunction exhibited optimal photocatalytic activity at 4.08 times and 1.57 times higher than those of pure CuO and SM-300, respectively, and excellent photocatalytic activity was detected in the peroxymonosulfate (PMS) system. Notably, metal and nonmetal ions in sediment themselves and 1 O 2 generated in PMS system are resistant to anionic and cationic interferences in water decontamination. In addition, the photocatalytic mechanism, possible intermediates, and degradation pathways were elucidated using theoretical calculations and experimental results. Moreover, mung bean sprout cultivation experiments confirmed the non-toxicity of the developed heterojunction and degraded tetracycline solution. These findings offer new insights to aid in synthesizing photocatalysts for wastewater treatment.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Jiajun Chen,Tiantian Yu,Gang Zheng,Wenhui Ma,Chaohui Wang,Xiaoxiao Huang,Shan Fan,Yong Zhang
Heteroatom doping and good porous structure play a decisive role in the energy storage characteristic of graphene-based supercapacitors. In this study, nanocellulose/N, S co-doped graphene composite hydrogel (NC-NSGHs) electrode materials were successfully prepared by a one-step hydrothermal method. During the reaction, ammonium sulfate was used as heteroatom source and reducing agent, nanocellulose (NC) was used as spacer and electrolyte storage container, and high a concentration of graphene oxide (GO, 4 mg mL −1 ) was used to increase the bulk density of the material. The target product NC-NSGHs have ideal pore structure, good hydrophilicity, and rich heteroatom functional groups. The aqueous symmetrical supercapacitors (SCs) assembled by NC-NSGH-50 exhibits high gravimetric specific capacitance (0.3 A g −1 , 280.6 F g −1 ), volumetric specific capacitance (0.3 A g −1 , 406.9 F cm −3 ), excellent rate performance (20 A g −1 , 81.06%) and superior cyclic performance. In addition, we added GO and NC into the PVA-KOH electrolyte system and developed a new gel electrolyte PVA-GN-KOH (PGNK). The flexible solid-state supercapacitors (FSSCs) fabricated by PGNK and NC-NSGHs display a high specific capacitance of 189.9 F g −1 (0.5 A g −1 ). Even at 20 A g −1 , the rate performance of the device can reach 60.24%. The emergence of NC-NSGHs and PGNK provides new ideas for high-performance portable supercapacitors.
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WATER RESEARCH
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2025
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IF 12.4
Cong Zhang,Zhipeng Zhang,Shuang Zhang,Yifeng Chen,Dunjie Li,Yongmei Li
Anaerobic co-digestion of sulfur-containing organic wastes with waste-activated sludge containing iron–phosphorus compounds (FePs) was recently suggested as an environment-friendly strategy to promote phosphate release, energy recovery, and hydrogen sulfide (H 2 S) control. Nevertheless, the mechanistic coupling between FePs speciation and the concurrent transformation of carbon, sulfur, iron, and phosphorus within this system remains to be fully elucidated. To address this knowledge gap, methionine, a typical hydrolysis product of sulfur-containing organics, and five FePs prevalent in sludge (ferric-phosphate tetrahydrate (FePO 4 ⋅4H 2 O), ferric-phosphate dihydrate (FePO 4 ⋅2H 2 O), vivianite (Fe 3 (PO 4 ) 2 ·8H 2 O), phosphate coprecipitated with Fe(III) (COP-P), and phosphate adsorption on hydrous ferric oxide (HFO-P)) were selected to elucidate C-S-Fe-P transformations in this study. The results showed that the H 2 S and methyl mercaptan productions decreased by >96% and >99%, respectively, while the methane production rate increased by 51.60–103.9% in the presence of FePs. The reaction between FePs and sulfide promoted the transformation of gaseous H 2 S and aqueous S 2− to solid sulfur species (elemental sulfur and iron sulfide precipitates), while simultaneously promoting the release of PO 4 3− from FePs. The formation of Fe(II) species derived from both abiotic sulfide-driven reduction and microbial-mediated iron reduction processes. The reduction rates of FePO 4 ⋅2H 2 O and FePO 4 ⋅4H 2 O were higher than those of COP-P and HFO-P, owing to their higher thermodynamic favorability. A negative correlation was observed between the Fe/P molar ratio and PO 4 3− release efficiency. FePO 4 (FePO 4 ⋅2H 2 O and FePO 4 ⋅4H 2 O) with the lowest Fe/P molar ratio achieved the highest P release efficiency (89.83–91.01%). Metagenomics analysis revealed that the SELENBP1 gene related to the degradation of methanethiol to sulfide was upregulated by 21.12–51.72% in the presence of FePs, and the genes involved in propionate metabolism, methylotrophic, and hydrogenotrophic methanogenesis were up-regulated concurrently. This study provides an in-depth understanding of C-S-Fe-P interactions and transformations during the anaerobic co-digestion of sulfur-containing organic wastes with FePs-containing sludge, helping to enhance methane production and the recovery of phosphorus and sulfur.
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