JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Hui Li,Ziqun Wang,Yunhui He,Sugang Meng,Yun Xu,Shifu Chen,Xianliang Fu
Rational synthesis of photocatalytic materials is an effective way to improve their performance. In this work, to optimize the S precursors, a series of Mn x Cd 1−x S (MCS) were first hydrothermally synthesized with the prevalent thiourea (TA), thioacetamide (TAA) and L-cysteine (L-Cys) as the S sources. The optimum feed ratio of Mn/Cd was then determined based on the optimized S precursor. The effects of S precursors and the feed ratio of Mn/Cd on the phase structure, absorption, morphology, band structure, and the photocatalytic hydrogen evolution reaction (HER) performance of MCS were investigated systematically. The hexagonal phase structures of MnS, CdS, and MCS are favored by TA and L-Cys as the S sources, while their cubic phases are benefited by TAA. TAA is the preferred S source for the preparation of highly active MCS and the solid solution is formed through the consolidation of cubic α-MnS into cubic CdS. The activity of MCS can be improved with the increase of Mn content from x = 0–0.6. The sample with x = 0.6 shows the highest HER activity (2253 μmol·h −1 ·g −1 ) and the performance is almost 6 times higher than CdS (416 μmol·h −1 ·g −1 ). The enhanced activity can be attributed to the improved separation efficiency of photo-induced charge carriers and the negative-shifts of E cb , which are induced by the introduction of Mn. A segregation of inert α−MnS from MCS is occurred when Mn content is >0.6, resulting in a decay of the HER activity. A change of the semiconductivity from n-type to bipolar type is occurred in MCS due to the uneven sulfidation of Mn in MCS.
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NEW JOURNAL OF CHEMISTRY
·
2025
·Vol. 49
·期 20
·8485-8493
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IF 2.5
Jiudi Zhang,Ruyu Zhang,Xiaowei Jia,Jinming Li,Mingliang Sun,Shikang Zhang,Zhenfu Guo,Xiaoyan Jiao,Xianchun Liu,Zhanshuang Jin,Junjie Li,Yan Xing
Tantalum nitride (Ta3N5) with suitable band structure and high theoretical solar-to-hydrogen energy conversion efficiency (15.9%) is regarded as one of the most promising semiconductor-based photocatalysts for hydrogen evolution via water splitting. However, it is practically constrained by the slow carrier mobility, fast electron–hole recombination and unabundant catalytic active sites. Herein, honeycomb-structured Ta3N5 foam nanoplates were successfully synthesized using a simple template-free strategy. It can not only capture broader visible light to generate the high concentration of photo-generated carriers, but also accelerate the rapid transport/separation of carriers and provide abundant active sites to accelerate the kinetics of water splitting reaction. Therefore, honeycomb-structured Ta3N5 exhibits excellent photocatalytic performance with a remarkably enhanced H2 production rate of 59.16 μmol h−1 g−1, which is 22.7 times higher than that of the conventional bulk Ta3N5. Moreover, the unique Ta3N5 with honeycomb structure has outstanding stability and recycling ability. This work provides a simple and effective strategy for the preparation of Ta3N5-based photocatalysts for efficient and stable H2 production.
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RENEWABLE ENERGY
·
2025
·
IF 9.1
Yu Zhang,Runzhe Li,Jingde Luan,Longde Jiang,Wengang Liu,Zheng Yan,Yu Bai
Photocatalytic hydrogen evolution from seawater splitting was a sustainable energy technology, alleviating the overuse of limited freshwater resources. The exogenous carbon was successfully doped into the framework of graphite carbon nitride via ultrasonic peeling and secondary calcination, replacing the bridging N atoms within the heptazine skeleton. This approach effectively regulated the chemical structure of g-C 3 N 4 , and the photocatalytic hydrogen yield of as-prepared CN-NA45 in water reached 7.15 mmolg −1 h −1 . In artificial seawater, the hydrogen yield of CN-NA45 increased to 10.80 mmolg −1 h −1 , which was attributed to the larger specific surface area, reduced band gap and more negative band edge. The presence of bridging carbon facilitated the transfer of electrons from the heptazine ring to the region near the bridging position, enhancing the local delocalization of π electrons. In artificial seawater, the adsorption of Na + ions on the catalyst surface were superior to other ions, facilitating the electron enrichment and providing more electrons for the photocatalytic reduction reaction. This work provided an insight into the construction of photocatalytic materials for marine environmental applications and the impact of electrolyte ions on hydrogen evolution performance.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2017
·
IF 9.446
Jia Cheng,Xiaojun Gu,Penglong Liu,Hao Zhang,Lunliang Ma,Haiquan Su
From the viewpoint of controlling the catalytic performance of supported metal nanoparticles (NPs) through tuning their chemical environment in the atom level, we have used electron-donating amino groups and three organic amine molecules to modify the organic linkers and unsaturated coordination Cr 3+ sites in one porous metal-organic framework MIL-101 with atomically precise structures, respectively, and then we have prepared a series of AuPd NPs immobilized by the two types of functional MIL-101 supports. The as-synthesized AuPd NPs were used for the catalytic dehydrogenation of formic acid (HCOOH) and the results showed that these catalysts exhibited remarkably different activities and H 2 selectivities at 298 K. Particularly, the AuPd NPs immobilized by MIL-101-NH 2 presented 100% of H 2 selectivity and the highest activity because of the synergistic steric and electronic effects, which were related to the activation of HCOOH and enrichment of electron density of active Pd species. The investigation of UV–vis spectroscopy showed that the reaction between the mixed metal ions (AuCl 4 − and PdCl 4 2− ) and the four functional MIL-101 supports generated four different coordination complex intermediates, which played an important role in yielding AuPd NPs with different chemical environment and inducing different catalytic performance.
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CERAMICS INTERNATIONAL
·
2026
·
IF 6
Chengkai Li,Changjian Zhou,Ze Liu,Zhenyu Zhang,Danni Zeng,Rongfeng Guan
Driven by the dual demands of global energy structure transformation and carbon neutrality goals, solar-driven green hydrogen and green chemical synthesis have become a focus. This study employs a Prussian blue template to guide the one-step synthesis of Cu/Ni co-doped Cd 0.9 Zn 0.1 S, which not only retains a high-surface-area porous framework with exposed active sites but also intentionally introduces abundant sulfur vacancies (Vs). The synergistic interplay of Cu doping (acting as electron-rich centers), Ni doping (serving as hole-trapping centers), and the generated V s collectively optimizes the band structure, extends light absorption to nearly 700 nm, and significantly enhances charge carrier separation. The optimized 10Cu/10Ni- Cd 0.9 Zn 0.1 S photocatalyst achieves an exceptional hydrogen production rate of 21.25 mmol g −1 h −1 (20-fold enhancement) and a H 2 O 2 production rate of 4.6 mmol g −1 h −1 under oxygen conditions (15-fold enhancement). Remarkably, the in-situ generated H 2 O 2 is efficiently activated on Cu/Ni sites and Vs via a photo-Fenton-like process, enabling rapid tetracycline degradation (94% within 40 min). DFT calculations reveal that the hydrogen adsorption free energy is optimized to −0.09 eV, and the introduced sulfur vacancies further lower the work function, promoting O 2 activation and charge transfer for both H 2 evolution and Fenton-like reactions. This study offers new insights into designing highly efficient photocatalysts by employing a coupled doping and vacancy engineering strategy to synergistically regulate redox-active sites, combining porous framework design for optimized mass transport and multifunctional environmental remediation.
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APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Pengcheng Wang,Jun Liu,Peiwen Xu,Xinzhen Feng,Weijie Ji
Three morphologically uniform γ-Al 2 O 3 crystallites [Al 2 O 3 hexagonal plates (Al 2 O 3 -HP), stacked hexagonal plates (Al 2 O 3 -SHP) and rods (Al 2 O 3 -R)] were controllably synthesized. The Co-Mo oxide precursor was loaded on these γ-Al 2 O 3 substrates via aqueous incipient wetness impregnation and transformed to the sulfides under 10% H 2 S/H 2 (v/v) atmosphere. The mainly exposed facet of Al 2 O 3 -HP and Al 2 O 3 -SHP was identified to be the (1 1 0) and (1 0 0)/(1 1 1), respectively; whereas a polycrystalline structure was observed over Al 2 O 3 -R. The original structural feature of oxide precursors, i.e., 2D polymeric/monomeric as well as 3D polymeric/MoO 3 species substantially varied over Al 2 O 3 -HP, Al 2 O 3 -SHP, and Al 2 O 3 -R, which in turn determines the effectiveness in sulfidation of surface oxide precursors. The richness of MoS 2 /Co 9 S 8 /Co-Mo-S species, and less fraction of partially sulphurated CoMoO x S 2 as well as CoO x /SO x 2− entities were recognized over Al 2 O 3 -HP. Based on the areal activity at 250 °C, the sulfides-Al 2 O 3 (1 1 0) interface is approximately 6–13.8 times more active than the poly-crystalline or commercial γ-Al 2 O 3 supported sulfides for water gas shift (WGS) in a hydrogen-rich stream. The sulfides-Al 2 O 3 (1 1 0) interface also notably outperformed the sulfides-Al 2 O 3 (1 0 0)/(1 1 1) interfaces for the reaction.
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JOURNAL OF MEMBRANE SCIENCE
·
2020
·
IF 7.183
Xiaochang Cao,Haoqing Xu,Songlin Dong,Jiayou Xu,Zhihua Qiao,Song Zhao,Jixiao Wang,Zhi Wang
In this work, we proposed a simple method to prepare high-performance and pressure-resistant mixed matrix membranes (MMMs) for CO 2 /H 2 separation. The groups or segments of poly-(vinylamine) (PVAm) were used to modify covalent organic frameworks (COFs), and COFs with similar frameworks but different surfaces were obtained. Then, modified COFs were mixed with PVAm matrix and used to coat the modified-polysulfone (mPSf) to prepare MMMs for CO 2 /H 2 separation. Modified COFs and the PVAm matrix were highly compatible because COF surfaces possessed the same groups or segments as PVAm. Meanwhile, in the coating solution, COF surfaces were found to induce penetration of PVAm molecules into COF pores, narrowing the pore size of the COFs and providing an amino environment for CO 2 preferential absorption and transport. The penetration degree was affected by the hydrogen bond between COF surfaces and the PVAm molecules. In addition, the incorporated COFs effectively restricted the mobility of the PVAm matrix, increasing the pressure resistance for MMMs under high pressure. In the gas permeation test, the optimal MMMs could achieve a CO 2 permeance of 957 GPU and a CO 2 /H 2 selectivity of 17.1 at 2.0 MPa because of the high compatibility and size of the channels (0.94 nm).
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JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Shuang Luo,Xingyan Liu,Xiangjun Wei,Min Fu,Peng Lu,Xuan Li,Yiming Jia,Qiao Ren,Youzhou He
The novel bifunctional NH 2 -MIL-125/Co(dmgH) 2 composite catalysts with several different Co(dmgH) 2 contents that can simultaneously achieve photocatalytic NO removal and hydrogen production were first prepared by a simple and convenient method. The corresponding physical and chemical properties of the composite catalysts were characterized by SEM, XRD, ESR, in situ DRIFTS, etc. The characterization results indicated that the noble-metal-free Co(dmgH) 2 , which was much cheaper and more available than most noble-metals such as Pt, could be an effective co-catalyst to accelerate the separation of photogenerated electron-hole pairs, further eventually enhancing the photocatalytic efficiency. Under visible-light irradiation for half an hour, the NO removal ratio of NH 2 -MIL-125/Co(dmgH) 2 (3 wt%) increased by 22.7 % compared with the pristine NH 2 -MIL-125 without Co(dmgH) 2 loading. In addition, it was found that Eosin Y dye-sensitized NH 2 -MIL-125/Co(dmgH) 2 (3 wt%) was capable of promoting a hydrogen generation rate of 2195 μmol g −1 h -1 under visible light, which was 12.6 times greater than the original NH 2 -MIL-125. This strategy was expected as an available way to fabricate noble-metal-free molecular complexes with metal-organic frameworks (MOFs) to enhance the photocatalytic NO removal and hydrogen production performance simultaneously.
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Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 17
·10543-10551
·
IF 10.733
Jin Song,Xiaojun Gu,Yaduo Cao,Hao Zhang
From the perspective of controlling visible-light-driven catalytic activities of supported metal catalysts by tailoring the band structures of semiconducting supports, we calcined pristine V2O5 in a H2 atmosphere at 250–350 °C to synthesize a series of porous two-dimensional V2O5 nanosheets with narrow bandgaps and rich oxygen vacancies, which supported Co and Ni nanoparticles as catalysts for visible-light-driven on-demand H2 evolution from ammonia borane (NH3BH3) in aqueous solution at 25 °C. The systematic investigations showed that all the catalysts had higher activities under visible light irradiation than in the dark and one Co catalyst exhibited the highest photocatalytic activity with a total turnover frequency (TOF) value of 120.4 min−1, which exceeded the values of all the reported noble metal-free catalysts. Structural characterization indicated that pristine V2O5 and the three post-modified V2O5 species had different bandgaps, valence band positions and concentrations of oxygen vacancies as well as different photocurrent densities, leading to different electron densities of active metal NPs in the supported catalysts with different catalytic activities. This was verified using the UV-vis spectra, valence band X-ray photoelectron spectroscopy, X-ray diffraction patterns and electrochemical characterization of various V2O5 species and the corresponding photocatalytic performance of catalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Heyu Li,Zhe Sun,Yan Cao
Gypsum (GP) by-products are a group of widely sourced sulfur-containing solid wastes and their recycling utilizations are of great significance. This work proposed a new cyclic GP utilization process, achieving both the sulfur recovery and simultaneous value-added syngas byproduct under the restriction of the CO 2 capture. This innovative process integrates the carbon-fueled and calcium-based chemical-looping technology to generate concentrated SO 2 , followed by the recovery of the sulfur to be a concentrating sulfuric acid via the iodine–sulfur thermochemical cycle and finally the CO 2 capture to produce CaCO 3 /(NH 4 ) 2 SO 4 by the use of the in-situ generating calcium adsorbent via the NH 3 -Merseburg process. Its feasibility was thermodynamically and experimentally validated. It’s found that the elevated temperature and the weak reducing atmosphere were conducive to a nearly 100% thermally-decomposed of GP (mainly CaSO 4 ) toward a mixture of CaS and CaO (a ratio in 4:6) and the maximum per pass carbon conversion over 80% using carbon fuels (coal), and the carbon residues can be recovered back to carbon fuel stream. The recovery of I 2 can be achieved through the electrochemical electrolysis method and then recycled. The optimization of heat exchange network results in energy consumption reduction by 79.6% and 75.2% for hot and cold utilities, respectively.
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INORGANIC CHEMISTRY
·
2026
·
IF 4.6
Lin Wei,Yang Zhibin,Tao Jin-Gang-Lu,Zhao Qianqian,Liu Fuyu,Li Wanshan,Feng Renfei,Zhang Yu,Fu Xian-Zhu,Luo Jing-Li,Zhao Bin
Developing efficient and durable electrocatalysts for
alkaline
seawater hydrogen evolution remains challenging because of sluggish
water dissociation kinetics. Herein, we report a defect-rich d-p orbital-hybridized
Os/o-CNTs electrocatalyst ( dph -Os def /o-CNTs)
prepared by rapid room-temperature NaBH 4 reduction. The
partially oxidized CNT support anchors defective Os nanoclusters and
induces C–Os/C–O–Os electronic coupling, generating
electron-deficient Os sites with modulated 5d electronic structures.
In alkaline simulated seawater (1 M NaOH + 3.5 wt % NaCl), dph -Os def /o-CNTs requires only 91 mV to reach
100 mA cm –2 and exhibits a Tafel slope of 19 mV
dec –1 , with stable operation over 350 h and 10,000
CV cycles. In situ Raman spectroscopy, AIMD simulations, and DFT calculations
reveal that Os vacancies reorganize interfacial water into an ordered
H-bond network, promote O-down water adsorption, and reduce the water
dissociation barrier from 1.12 to 0.56 eV. Moreover, an Al | OH – | H 2 primary cell using dph -Os def /o-CNTs as the cathode delivers 1.41 V and 10.92
mW cm –2 , enabling simultaneous hydrogen generation
and electricity output.
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JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Da Wang,Yinning He,Na Zhong,Zhiqiao He,Yi Shen,Tao Zeng,Xiaohui Lu,Jun Ma,Shuang Song
This study investigated the simultaneous photoelectrochemical (PEC) degradation of carbamazepine (CBZ), reduction of CO 2 and production of H 2 using a TiO 2 thin film as photoanode and Ag plate as cathode . The photoanode was fabricated using sequential hydrothermal and calcination processes. The use of chloride during the hydrothermal process enhanced formation of oxygen vacancies and defects on the TiO 2 surface. Calcination not only further strengthened those features but also enhanced the crystallinity and anatase/rutile ratio, endowing the TiO 2 photoanode with superior PEC capacity. Characterization of physicochemical and PEC properties revealed that photogenerated electrons-holes were rapidly generated and efficiently separated on the TiO 2 surface during the PEC process. Hydroxyl radicals were the main active species responsible for anodic oxidation of carbamazepine, while hydrogen radicals and carbon dioxide radical anions mediated CO 2 reduction and H 2 production in the cathodic process. This work confirms the suitability of the prepared TiO 2 photoanode for PEC degradation of organic pollutants coupled with CO 2 reduction and H 2 production.
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