PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2022
·
IF 7.926
Haoran Leng,Zhiying Lv,Haili Tan,Yuhong Jia,Hong You
As a representative pollutant with carcinogenesis, mutagenicity and teratogenicity , nitrobenzene (NB) has devastating harm to human health. Herein, a unique three-dimensional (3D) stack Z-scheme photoelectrocatalytic (PEC) system was built by self-assembled different photoelectrodes for efficient NB removal. The effect of initial NB, bias potential, pH and electrolyte concentration on NB removal efficiency were investigated. The intermediates and oxygen-active radicals were determined and analyzed by high performance liquid chromatography (HPLC), gas chromatography-mass spectrometry (GC-MS), density functional theory (DFT) and electron paramagnetic resonance (EPR) to propose the NB degradation pathways and mechanism. The results showed that holes were utilized to produce ·OH to oxidize NB on the photoanode surface, the electrons excited from photocathode could reduce NB under UV irradiation; thereafter, the reduction product (aniline) was oxidized to phenol to achieve mineralization by the synergistic effect of anode (oxidation) and cathode (reduction). 3D stack Z-scheme PEC system exhibited a high NB degradation efficiency of 98.18% after 90 min reaction and a mineralization efficiency of 75.08% at 150 min. With ECOSAR software, the system toxicity was speculated. This study has advantages in NB removal and provides direction for other refractory organics.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CONTROLLED RELEASE
·
2026
·
IF 12.4
Jianhua Liu,Bingru Shao,Qiannan Miao,Jin Wang,Zhihua Wang,Mingda Han,Yuchuan Hou,Fei Yan
Sonodynamic therapy (SDT) provides spatially controlled tumor treatment, but its efficacy in hypoxic tumors is limited by oxygen-dependent reactive oxygen species (ROS) generation and tumor-associated macrophage (TAM)-mediated immunosuppression. Here, we developed a hyaluronic acid (HA)-modified, metal–organic framework (MOF)-based CuO₂@FeTCPP Z -scheme nanosonosensitizer to combine hypoxia-tolerant hydroxyl radical (•OH) generation with macrophage reprogramming. Band-edge analysis, interfacial X-ray photoelectron spectroscopy, and spin-trapping and scavenging experiments provided complementary support for a Z -scheme charge-transfer pathway that preserves reducing electrons on FeTCPP and highly oxidative holes on CuO₂. Under ultrasound irradiation, CuO₂@FeTCPP@HA maintained strong •OH generation under hypoxia, whereas oxygen-dependent 1 O₂ production was substantially attenuated. HA modification enhanced CD44-associated cellular uptake, as demonstrated by comparison with the HA-free material and by CD44-blocking experiments. In M2-like macrophages, CuO₂@FeTCPP@HA treatment without ultrasound was accompanied by increased H3 acetylation and decreased H3K9 trimethylation, whereas ultrasound activation markedly increased •OH production and amplified the M2-to-M1 phenotypic and cytokine responses. These observations support distinct but convergent contributions from Cu-associated metabolic–epigenetic regulation and ultrasound-triggered oxidative stress. In a bilateral subcutaneous A20 lymphoma model, local treatment of the primary tumor suppressed both irradiated primary and non-irradiated contralateral tumors, reduced the bone marrow lymphoma burden, and promoted dendritic cell maturation, CD8 + T-cell infiltration, and effector memory T-cell formation. Together, these results demonstrate a materials-based strategy that integrates oxygen-independent sonocatalysis with macrophage-centered immune remodeling for systemic antitumor therapy. Download: Download high-res image (621KB) Download: Download full-size image
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2023
·
IF 4
Shuang Wang,Mengjie Yao,Yuye Cheng,Kai Ding,Minghao Dou,Hongyu Shao,Shuaitong Xue,Shenjie Li,Yanyan Chen
By providing the spatial separation of the active sites and retaining high oxidative and reducing capacity, the direct Z-scheme heterostructure is considered the most potential structure for yielding photo-electric response. However, challenges still exist in the directional transfer of charge carriers between two semiconductors in direct Z-scheme structures. In this regard, by constructing the Vzn defect and p–n junction, a direct Z-scheme ZnxCd1−xS@ZnS-NiS heterostructure was obtained for the regulated electronic structure, which ensured high-yield hydrogen properties. The Zn vacancy in the partially-coated ZnS shell led to the Vzn energy level, and the addition of NiS led to the p–n structure, which caused a drastic downshift of the band edge potentials in comparison to that of pristine CdS. This variation gave rise to a staggered band edge alignment between ZnxCd1−xS and NiS, resulting in the variation of charge transfer kinetics from type-I to direct Z-scheme. Through careful characterization, it was found that the optimal photocatalytic hydrogen precipitation activity reached 16 683.6 μmol g−1 h−1, which was 70 times that of CdS, and this improvement was considered to form a spatial barrier, providing a clear direction and path for carrier transmission.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2023
·Vol. 99
·期 2
·415-425
·
IF 3.4
Mingliang Chen,Guanghui Wang,Jialing Dai,Haifeng Li,Nansheng Deng
BACKGROUND There is increasing concern regarding the rising issue of Cr(VI) pollution in aqueous solutions. It is crucial to find an effective technology for the removal of Cr(VI) in aqueous solutions. In this work, a novel TiO 2 /BC/g-C 3 N 4 heterostructure photocatalyst was successfully prepared by a simple hydrothermal method and characterized by scanning electron microscopy, transmission electron microscopy, X-ray diffraction, Brunauer–Emmett–Teller analysis, Fourier transform infrared spectroscopy, photoluminescence, ultraviolet–visible diffuse reflectance spectroscopy and X-ray photoelectron spectroscopy. The photocatalytic reduction behavior of Cr(VI) on the TiO 2 /BC/g-C 3 N 4 heterostructure was investigated under visible light irradiation, and the possible mechanism of photocatalytic reduction of Cr(VI) was elucidated. RESULTS The TiO 2 /BC/g-C 3 N 4 heterostructure photocatalyst exhibited better photoreduction activity for Cr(VI) under visible light irradiation. After 100 min irradiation with visible light, the TiO 2 /BC/g-C 3 N 4 photocatalyst achieved a removal efficiency of 89% for Cr(VI). Compared with TiO 2 , TiO 2 /BC and TiO 2 /g-C 3 N 4 , the photocatalytic removal efficiency of Cr(VI) on the TiO 2 /BC/g-C 3 N 4 increased by 40%, 20% and 10% respectively. The photocatalytic reduction of Cr(VI) was dependent on the initial concentration of Cr(VI), catalyst dosage, pH value and atmosphere. Moreover, TiO 2 /BC/g-C 3 N 4 presented excellent stability and reusability after five cycles. CONCLUSION The TiO 2 /BC/g-C 3 N 4 heterojunction enables highly efficient photocatalytic reduction of Cr(VI) under visible light irradiation. This enhancement is primarily attributed to the construction of an indirect Z-scheme TiO 2 /BC/g-C 3 N 4 heterojunction, which significantly improves the separation efficiency of photo- generated charge carriers during the photochemical process. Furthermore, the presence of BC enhances the adsorption performance of Cr(VI) on TiO 2 /BC/g-C 3 N 4 , thereby facilitating its photocatalytic reduction. © 2023 Society of Chemical Industry.
✓ 已验证
产品关联
DOI
高影响因子
Polymer Chemistry
·
2016
·Vol. 7
·期 22
·3756-3765
·
IF 5.687
Mingguang Yu,Jianbo Tan,Jianwen Yang,Zhaohua Zeng
In a common RAFT dispersion polymerization induced self-assembly (PISA) formulation, R-type macro-RAFT agents with a solvophilic chain attached at the leaving group side are normally used to mediate the polymerization, meanwhile Z-type macro-RAFT agents with a solvophilic chain attached at the Z-group side are seldom employed. In this paper, we have tried to use a Z-type macro-RAFT agent (mPEG113-BTPA) to mediate RAFT dispersion polymerization of styrene, and found that the process exhibited a poorer PISA tendency and weaker molecular weight control. In comparison, we have conducted the same process mediated with an R-type macro-RAFT agent (mPEG113-DDMAT), and found that the formulation exhibited a typical PISA process, and nanoparticles were produced in situ. Further experiments suggest that the location of RAFT groups plays a key role for the PISA process in RAFT dispersion polymerization. The RAFT groups will be embedded in the produced particles when an R-type macro-RAFT agent is employed, but locate on the particle surface in the case of the Z-type macro-RAFT agent. We have tried to employ the RAFT groups on the surface of the mPEG113-BTPA stabilized particles to modify the particle surface, and successfully removed the solvophilic block via breaking the RAFT group, and generated the poly(dimethylacrylamide) block by surface-initiated RAFT polymerization. Based on the above mechanism perspective, we have designed a preliminary experiment, and found that well-defined monodisperse nanospheres could be prepared by heterogeneous RAFT dispersion polymerization mediated with a Z-type macro-RAFT agent-based block copolymer which was synthesized via pre-polymerization of styrene in 1,4-dioxane mediated with mPEG113-BTPA.
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Shuaishuai Liu,Junhao Jiang,Chengzhao Jin,Ruixve Sun,Zengming Man,Pengxin Li,Kun Chang
Constructing Z-scheme heterojunctions by establishing a unique charge transfer pathway at the interface has garnered growing attention in photocatalytic technology. In this study, a p-n heterojunction of Z-scheme was developed by employing an in-situ annealing strategy following the electrostatic self-assembled chemistry, with n-type ZnO and p-type Bi 2 O 3 as the constituent materials. Upon AM 1.5 G irradiation, the optimal ZnO/Bi 2 O 3 (Zn/BO) photocatalysts achieved a remarkable H 2 -evolution reaction (HER) rate of 458.3 μmol∙h −1 , which was 10.5 times higher than that of the original ZnO and 5 times higher than that of Bi 2 O 3 , respectively. Moreover, its efficiency in degrading 100 mg∙L −1 rhodamine B (RhB) reached 100% within a 60-minute period. Its rate constant was 24.70 and 11.71 times higher compared to ZnO and Bi 2 O 3 , respectively. The proposed Z-scheme mechanism of electron transfer was put forward to explain the observed enhancement in photocatalytic performance, as determined by in-situ XPS experiments. Furthermore, the Zn/BO photocatalyst exhibited exceptional catalytic activity when exposed to visible light (λ > 420 nm). The remarkable cycle stability of the hollow Z-scheme catalyst further suggests its potential for facilitating the industrialization of photocatalytic technology.
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2023
·Vol. 13
·期 21
·6198-6210
·
IF 5
Jun Pang,Weijie Chen,Jintao Hu,Jie Cheng,Mingqiang Tang,Zewei Liu,Rong Tan
Metal–organic frameworks (MOFs) have emerged as promising photocatalysts due to their tunable architectures and semiconductor-like behavior. However, their photocatalytic efficiency is often hampered by suboptimal light utilization and fast charge carrier recombination. To address these challenges, we developed core–shell MOF@COF Z-scheme hybrids, where a covalent organic framework (COF, TpBD-COF) was coated on the NH2–UiO-66 surface via imine bond interconnection. Characterization and DFT calculation results suggested the formation of a well-contacted interface, as well as a Z-scheme heterojunction between the NH2–UiO-66 core and TpBD-COF shell. The TpBD-COF shell with an inherently narrow energy band contributed to the visible light absorption, while the fabricated Z-scheme heterojunction resulted in the spatial electron–hole (e−–h+) separation and high redox ability. By rationally controlling the ratio of NH2–UiO-66 and TpBD-COF precursors, the tailored thickness of the TpBD-COF shell was achieved, which could modulate the Z-scheme heterojunction interface, and thus optimized the photocatalytic performance. The core–shell MOF@COF hybrids were highly efficient in visible light-driven oxidative coupling of amines to imines in air without the need for any sacrificial agents. Almost quantitative conversion (94%) of benzylamine to N-benzylidenebenzylamine was achieved over optimal NH2–UiO-66@TpBD-COF(21.9), which is approximately 4.0 and 1.5 times that of pristine NH2–UiO-66 and TpBD-COF, respectively. The superior catalytic performance, coupled with benign reaction conditions (visible light, room temperature, ambient air), makes NH2–UiO-66@TpBD-COF(x) highly promising for solar utilization in green synthesis.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Jinghao Hua,Changchang Ma,Dayu Wu,Haitao Huang,Xiaojun Dai,Kaidi Wu,Haihong Wang,Zhaowei Bian,Sheng Feng
In this study, a novel Z-scheme Bi 19 S 27 Br 3 /CoAl-LDH heterojunction was prepared. An interface charge transfer channel was established between Bi 19 S 27 Br 3 and CoAl-LDH, accelerating the transition efficiency of interface electrons from CoAl-LDH to Bi 19 S 27 Br 3 . Thereby ensuring more excited electrons to participate in CO 2 photoreduction reactions. The reduction products were tested under artificial light conditions, and triethanolamine was selected as a sacrificial agent. After 5 h of illumination, the CO yield of Bi 19 S 27 Br 3 /CoAl-LDH Z-scheme heterojunction was 86.41 μmol·g −1 is 4 times and 7 times higher than Bi 19 S 27 Br 3 and CoAl-LDH, respectively. The yield of CH 4 in Bi 19 S 27 Br 3 /CoAl-LDH is 3.97 μmol·g −1 is 4 times higher than CoAl-LDH. Also Bi 19 S 27 Br 3 itself does not produce CH 4 . The results indicate that the Z-scheme heterojunction effectively enhances the photoreduction ability of CO 2 , providing a new approach for accurately controlling the direction of photo generated charge separation to prepare high-performance photocatalysts.
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Hui Chen,Xin Yang,Min Lin,Dongmiao Li,Bing Wang,Jinni Shen,Jinlin Long,Wenxin Dai,Xuxu Wang,Zizhong Zhang
Mimicking natural photosynthesis to convert CO2 and H2O into highly valuable solar fuels is one of the ideal ways to alleviate the energy shortage and environmental pollution. However, the low mobility of photogenerated holes and sluggish H2O oxidation half reaction seriously retard the reduction efficiency of CO2 by photocatalysis. In this paper, we reported that the visible light-active SiC photocatalyst was inserted into the InVO4 nanoflower framework to form the dual Z-scheme heterojunction composited photocatalyst. The composited photocatalysts can not only neutralize the low mobility of photogenerated holes on SiC but also improve the H2O oxidation on InVO4 nanoflowers. This leads to an effective conversion of CO2 to CO without sacrificial agents under visible light irradiation as well as a good separation of photogenerated charge carriers in the composited photocatalyst for the subsequent reaction. In comparison to the parent InVO4 and SiC, the optimum CO yields over InVO4/SiC were 9.41 and 11.54 times, respectively. Under 3 h visible light irradiation, the yields of CO reach up to 142.6 μmol·g–1 and stability of O2 release over InVO4/SiC. This research offers a practical approach to developing an efficient photocatalyst for the conversion of CO2 with H2O.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2023
·
IF 6.1
Feihu Zhang,Xinyan Xiao,Yu Xiao,Xia Cheng
An innovative 3D flower-like BiOI/Bi 3 O 4 Br hierarchical heterostructures complex material was firstly constructed via in-situ growth of ultrathin BiOI on Bi 3 O 4 Br by a simple precipitation method. Under the simulated solar-light illumination for 90 min, the optimal 60% BiOI/Bi 3 O 4 Br composite displayed the highest photodegradation rate of 96.4% for RhB, 80.0% for TC and 77.2% for MO. The corresponding apparent rate constants were 0.0314, 0.0167 and 0.0110 min −1 , which were 8.26, 1.82 and 3.24-times than that of Bi 3 O 4 Br, 44.86, 11.13 and 2.62-times than that of BiOI. The improved photodegradation activity could be owing to the following reasons: 1) The 3D hierarchical heterostructures endowed BiOI/Bi 3 O 4 Br with tight interfacial contact, which can supply sufficient migration channels for photoinduced carriers; 2) The Z-scheme charge migrate pathway promoted the segregation of photocarriers while maintaining a robust redox ability; 3) The BiOI/Bi 3 O 4 Br heterostructures reinforced light absorption edges more than 600 nm and augmented specific surface areas over 60 m 2 ·g −1 . In addition, the various photocatalytic conditions were studied to imitate the degradation process of RhB in the real aqueous system. The radical capture experiments and EPR test attested that h + and O 2 − played an important part in the photodegradation of RhB.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Jie Cui,Lin Ye,Xiaoxi Chen,Jianing Li,Bian Yang,Man Yang,Qing Yang,Daqin Yun,Shaodong Sun
Exploring novel materials with both high adsorption capacity and photocatalytic properties is urgent in environmental remediation. In this work, a Z-scheme ZnO/Cu 2 O heterostructure with a large surface area of 45.42 m 2 /g was constructed by using the liquid phase reduction method. Compared to pure ZnO and pure Cu 2 O, the as-synthesized ZnO/Cu 2 O nanocomposites exhibited excellent capacity of adsorption and photodegradation for tetracycline (TC), which was degraded 95.3% of TC within 120 min under simultaneous adsorption and photocatalytic processes. Theory and experimental analysis manifested that the excellent adsorption-photocatalytic activity can be attributed to the large BET specific surface area, the efficient charge carrier separation and the high redox capability. The results of this study identified the potential advantages of ZnO/Cu 2 O composites for removing antibiotics to purify water resources and protect the environment.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jingwen Wei,Ting Liang,Shiming Zhang,Jinhang Yang,Zhihong Li,Zuji Li,Songyu Fan,Zebin Yu,Yanping Hou
In this work, the Z-scheme layered double hydroxide (LDH)/reduced graphene oxide (RGO)/indium vanadate (InVO 4 ) heterojunction was synthesized by a simple hydrothermal synthesis. RGO , with excellent electron mobility, endowed rapid charge migration and separation between the CoAl-LDH and InVO 4 . Various characterizations and tests showed that the LDH/RGO/InVO 4 heterojunction exhibited superior optical properties, and its carriers’ transfer pathway conformed to Z-scheme mechanism. Under visible light illumination, CO was observed to be the main product during photocatalytic CO 2 reduction, and the LDH/RGO/InVO 4 -15 exhibited the highest CO yield of 204.86 μmol g −1 within 2 h, approximately 2.62 times of pristine CoAl-LDH (78.2 μmol g −1 ). In addition, LDH/RGO/InVO 4 -15 showed favorable structure stability and performance stability. In situ fourier infrared spectroscopy (ISFT-IR) analysis demonstrated that the predominant intermediates of CO 2 reduction process were carboxylate (COOH*) and bicarbonate (HCO 3 *). Accordingly, possible pathways of CO 2 reduction to CO were deduced. This work can advance the development of efficient Z-scheme heterojunction photocatalysts for CO 2 reduction.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）