Journal of Physical Chemistry C
·
2019
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IF 4.309
Yongke Zhang,Zhiliang Jin
g-C3N4@ZIF-67 composite photocatalyst-supported NiSx are successfully prepared by a hydrothermal method using g-C3N4 and ZIF-67 as carriers. The synthesized composite catalyst has an efficient photocatalytic H2 production effect. Under visible light irradiation, the maximum H2 production within 5 h over the [g-C3N4@ZIF-67/(10%wt)NiSx] photocatalyst is 208 μmol, which is 8.32 times higher than that of pure g-C3N4. Based on the analysis of scanning electron microscopy and transmission electron microscopy, it is not only known that g-C3N4 and ZIF-67 provide space for the loading of NiSx nanoparticles but also that ZIF-67 as a carrier framework can effectively reduce the particle size of NiSx nanoparticles and increase the dispersion of NiSx. Further studies of photoluminescence (PL), time-resolved PL, i–t, linear scanning voltammetry, electrochemical impedance spectroscopy, and Mott–Schottky curves, we can not only know that the modification of NiSx nanoparticles do enhance the electron transfer ability but also that the matched conduction band position between g-C3N4 and ZIF-67 provides a feasible thermodynamic path for the transmission of electrons. Based on the DFT calculations, both NiS2 and Ni3S4 show the metallic characteristics, which means the outstanding electrical conductivity of them and implies the excellent capability to transport electrons. The work function of NiSx with metallic properties is more negative than that of the semiconductor, which indicates that the loading of NiSx can further promote the separation of electrons, thereby improving the H2 production efficiency.
研究领域:
材料科学
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能源化学
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催化科学
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
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IF 7.392
Xiaobin Dong,Han Wang,Xiaolong Li,Pedram Fatehi,Shoujuan Wang,Qin Wu,Keyin Liu,Fangong Kong
Graphitic carbon nitride is a very potential photocatalytic catalyst for H 2 production, but its practical application is seriously limited by the fast recombination of photogenerated carriers and insufficient utilization of surface charge. In order to solve these problems, herein, a series of g-C 3 N 4 -NiO-NiS x photocatalysts were synthesized by first calcining the precursor to load NiO on g-C 3 N 4 and subsequently partial sulfidation of NiO into NiS x in situ via a hydrothermal process. Under the irradiation of visible light, the photocatalytic H 2 production rate of g-C 3 N 4 -NiO-0.4T can be up to 1248.1 μmol·g −1 ·h −1 using triethanolamine as sacrificial agent. In addition, recycling test also confirmed g-C 3 N 4 -NiO-0.4T has excellent photostability. It is believed that the formation of p-n junction between NiO and g-C 3 N 4 and the presence of NiS x promote the spatially fast separation of photogenerated carriers, while the abundant interface of NiS 2 and NiS also leads to the good proton trapping ability. These two factors jointly determine the efficient H 2 production of the composite photocatalysts. Furthermore, the detailed energy band structure and plausible photocatalytic mechanism of g-C 3 N 4 -NiO-NiS x are also proposed. This work can offer a new route and useful reference for the design and research of high efficiency composite photocatalysts for H 2 production.
研究领域:
材料科学
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能源化学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
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IF 6.3
Huansheng Liu,Hanhan Lv,Chihao Lu,Yi Zhang,Daniel K. Macharia,Zheng Tang,Zhigang Chen
Traditional photocatalysts are usually prepared in first-pot and then dried, and re-dispersed in the second-pot for photocatalytic H 2 generation, where the two-pot mode may lead to loss/underutilization of active sites. To maximize active sites, herein we propose in-situ synthesis and photocatalytic hydrogen (H 2 ) evolution in one-pot mode. NiS x -modified Cd x Zn 1-x S (NiS x -CZS) photocatalysts as a model are prepared by photochemical reactions of metal salt precursors in the presence of sulfur. Among NiS x -CZS photocatalysts, 2 wt% NiS x -CZS exhibits the strongest photoabsorption in the visible region and the highest photocurrent response, implying that it produces the most photoexcited electrons under visible light irradiation. When irradiated by visible light (≥ 420 nm), the in situ H 2 generation rate of optimized 2 wt% NiS x -CZS with higher concentration of active sites is 17.98 mmol g -1 h -1 (one-pot mode), which is better than the two-pot mode (15.08 mmol g -1 h -1 ). Besides, the presence of in situ attached NiS x co-catalyst on CZS host results in a 22.2-fold H 2 production rate compared to pristine CZS. H 2 production performance with NiS x co-catalyst (89.92 mmol g -1 ) within 5 h is also better than noble/transitional metals as co-catalysts (9.62-26.99 mmol g -1 ). The amorphous NiS x provide sufficient unsaturated edge sulfur (S) sites, which serve as active centers to capture and enrich H + and lead to the expedited H 2 generation through the effective combination of H ads atoms. This work provides a unique insight into the one-pot photochemical synthesis of photocatalysts with charge-accumulated active sites and a rational strategy for in situ hydrogen production.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
DALTON TRANSACTIONS
·
2018
·Vol. 47
·期 36
·12671-12683
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IF 4.099
Sugang Meng,Yanjuan Cui,Hao Wang,Xiuzhen Zheng,Xianliang Fu,Shifu Chen
The development of stable noble metal-free photocatalysts with efficient separation and transportation of the photogenerated electrons–holes is of crucial importance for promoting the application of photocatalysis technology. Herein, we propose an electron transfer strategy by reasonable design and fabrication of novel 0D NiSx nanosheets as a co-catalyst on the surface of 1D CdS nanorods (CdS-NRs) to enhance photocatalytic hydrogen evaluation and contamination (Cr(VI), rhodamine B and bisphenol A) removal in water. Under visible light irradiation, the 0D–1D NiSx/CdS-NR nanocomposite with 1.5% NiSx loading gave a hydrogen evolution rate of 5.98 mmol h−1 g−1, which is about 5.3 times and 1.9 times higher than that of the native CdS-NRs and the optimal 1% Pt/CdS-NRs, respectively. Notably, good stability in the recycling test and a high apparent quantum efficiency of about 69.9% at 420 nm were also obtained. The 1.5% NiSx/CdS-NRs exhibited enhanced photocatalytic contamination degradation efficiency of about 2 times higher than pure CdS-NRs. In this hybrid photocatalyst, 0D NiSx nanosheets came into intimate interfacial contact with the surface of 1D CdS-NRs and played a similar role as noble metals, which could effectively improve the separation, transportation efficiencies and lifetime of photogenerated charge, and thus enhance the photocatalytic performance of CdS-NRs with more efficient conversion of solar energy. This work shows not only a possibility for the utilization of noble metal-free NiSx as a co-catalyst in the photocatalysis, but also provides new insight into the design and fabrication of high-performance composite photocatalysts (such as NiSx/g-C3N4 and NiSx/Zn3In2S6).
研究领域:
材料科学
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环境科学
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能源科学
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产品关联
DOI
PubMed
高影响因子
FOOD CHEMISTRY
·
2024
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IF 8.5
Jing Zhang,Jing Chen,Jincen Zuo,Jingsha Lan,Zhilin Jiang,Chen Xiao,Xinhui Wang,Yong Zuo
Excess nitrites are potentially threatening to human health, so it is urgent to develop accurate and sensitive methods. The development of sensors can provide early warning of possible hazards and alert people to protect public health. This work presents an NiS x @MoS 2 -composite with excellent electrochemical activity, representing a key finding for highly sensitive NO 2 − detection and sensor development. With the assistance of NiS x @MoS 2 , this electrochemical sensor has excellent quantitative detection performance. It has a wide detection range (0.0001–0.0020 mg/mL) and a low detection limit (1.863*10 −5 mg/mL) for NO 2 − . This electrochemical sensor maintains excellent specificity among numerous interferences, and it completes the accurate detection of different real food samples. Pleasingly, the electrochemical sensor has satisfactory repeatability stability, and potential for practical applications. It would demonstrate tremendous potential in scientific dietary guidance, food safety detection and other fields.
研究领域:
分析化学
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环境科学
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食品安全
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产品关联
DOI
PubMed
高影响因子
Materials Advances
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2021
·Vol. 2
·期 12
·3881-3891
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IF 0
Shenglong Gan,Min Deng,Dongfang Hou,Lei Huang,Xiu-qing Qiao,Dong-sheng Li
Optimization of cocatalysts is promising and of great significance in enhancing photocatalytic H2 generation from the perspective of understanding the charge separation, surface reaction kinetics, and distribution of active sites. Herein, we synthesize a class of well-formed hybrid photocatalysts by coupling amorphous NiSx films to ultrafine ZnCdS nanoparticles for greatly boosting the photocatalytic activity as well as the outstanding stability and repeatability. Under visible-light irradiation, the highest H2 evolution rate of the as-synthesized NiSx/ZnCdS photocatalyst achieved is 67.75 mmol g−1 h−1, which is 28.8 times higher than that of Pt/ZnCdS. Further detailed characterization reveals that the amorphous NiSx film as an excellent cocatalyst not only improves the spatial separation of the photoinduced carriers but also collects electrons and enlarges the reduction reaction space. This work could provoke interest in understanding the spatial charge migration in the cocatalyst system with an amorphous film structure, thus developing high-performance low-cost composite photocatalysts for H2 production.
研究领域:
材料科学
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能源化学
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DOI
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Xinlei Zhang,Fei Wu,Guicun Li,Lei Wang,Jianfeng Huang,Alan Meng,Zhenjiang Li
Photocatalytic water splitting is a prospective approach to address the energy and environmental challenges. Herein, an amorphous Ni@NiS x cocatalyst has been fabricated and simultaneously assembled onto CdS to form amorphous-crystalline Ni@NiS x -CdS photocatalyst via a partial reduction strategy. Comprehensive experiments and theoretical calculations demonstrate that the synergistic effects between the electronic coupling of amorphous-crystalline interface and the gradient work function variation induced by Ni nanocluster encapsulation achieve the deeper downshift of the S p-band center to optimize H* intermediate adsorption, enhance charge extraction ability though Schottky junction and lower H* adsorption Gibbs free energy (ΔG H* ). Accordingly, the optimal Ni@NiS x -CdS photocatalyst delivers a remarkable photocatalytic H 2 production rate of 78.7 mmol·g −1 ·h −1 with an apparent quantum efficiency (AQE) of 36.74% at 420 nm, which is approximately 18.3 and 1.5 times than that of CdS and NiS x -CdS, respectively. This work offers a novel insight into the development of amorphous nanocomposite cocatalysts for promoting solar-to-H 2 energy conversion.
研究领域:
材料科学
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能源化学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Guoqiang Zhang,Jianqing Li,Zhiqi Wang,Xi Xu,Tao He,Jingli Wu,Jinhu Wu
The cocatalysts play a key role in photocatalytic technology in remarkably improving the efficiency of H 2 evolution. Herein, S vacancies-rich Cd 0.6 Zn 0.4 S nanorods (CZS NRs) were prepared via solvothermal method. Then, as-obtained CZS NRs were modified with Ni–Co PBA-derived NiS x nanoparticles (NPs) cocatalyst using grinding method. The optimized CZS/NiS x -N-1.5 hybrids (CZS/NiS x -N, where N represents nickel nitrate which was used as nickel source) exhibited outstanding stability and activity, the average rate of H 2 was up to 192.82 mmolg −1 h −1 in deionized water medium, which was 201.4% higher than that of CZS. Besides, NiS x -A and NiS x -C cocatalysts with different particle sizes were obtained using nickel acetate (A) and nickel chloride (C) as nickel source, respectively. The CZS/NiS x -C-1.5 and CZS/NiS x -A-1.5 exhibited the H 2 evolution rate of 180.70 and 201.93 mmolg −1 h −1 in deionized water medium, respectively. The as-prepared materials also exhibited the excellent H 2 evolution performance in natural seawater medium. Besides, the photocatalytic mechanism of H 2 evolution over CZS NRs/NiSs NPs was also discussed. This work develops a novel H 2 evolution cocatalyst and unveils the relationship between the loading amount/particle size of cocatalyst on the H 2 evolution rate.
研究领域:
材料科学
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能源科学
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DOI
高影响因子
GREEN CHEMISTRY
·
2021
·Vol. 24
·期 2
·877-884
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IF 10.182
Baolong Zhang,Hui Fu,Tiancheng Mu
Electrochemical oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) has drawn wide attention recently. Rational interface engineering can modulate the electronic structure, tune the adsorption energy and endow the hybrid material with more active sites for HMF electrochemical oxidation. Herein, we propose a strategy for the synthesis of metal sulfide/metal phosphide (MSx/MPy, M = Co, Fe, Ni…) nanotube arrays with abundant interfaces by the sequential electrodeposition interface engineering method. Since Ni-based electrocatalysts show high efficiency for the electrochemical oxidation of HMF, we designed and synthesized interface-rich heterogeneous NiSx/Ni2P nanotube arrays. The abundant interfaces promote electron transfer between NiSx and Ni2P, which synergistically improves the oxidation state of the Ni species and further enhances the electrocatalytic performance of HMF oxidation. The NiSx/Ni2P electrocatalyst shows superb HMF oxidation activities with a low onset potential of 1.25 V vs. RHE. A current density of 20 mA cm−2 can be reached at 1.346 V vs. RHE, which is reduced by 204 mV compared with that with water oxidation. Chronoamperometry electrolysis reveals that HMF conversion is nearly 100% and FDCA selectivity can reach 98.5%.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2026
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IF 4.6
Fan Lin,Shaojie Lei,Jian Yang,Zichen Li,Hui Zhang,Zhibao Huo,Dezhang Ren
The electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) represents a pivotal step in facilitating the industrialization of bio-based polyesters. While nickel sulfides are widely regarded as promising electrode materials for HMF oxidation (HMFOR), systematic research regarding their structural stability under anodic conditions and the identification of their true active species remains insufficient. Herein, we employ cyclic voltammetry (CV) pretreatment as a controllable strategy to investigate the electrochemical oxidative reconstruction of NiS x in an alkaline environment by regulating the upper-potential (ranging from 0.9–1.4 to 0.9–1.8 V vs. RHE). This approach elucidates the structure-activity relationship between the degree of reconstruction and HMFOR performance. The results demonstrate that NiS x undergoes surface sulfur oxidation even at relatively mild potentials. As the upper potential increases, the initial spherical structure gradually reconstructs into NiO x -rich nonosheet structures, accompanied by an increased population of Ni 3+ species, accelerated charge transfer kinetics and significantly enhanced electrochemically active surface area. Specifically, moderate reconstruction (e.g., at an upper potential of 1.7 V) achieves an optimal balance between structural stability and the abundance of Ni 3+ active sites, thereby yielding superior HMF conversion efficiency and FDCA selectivity. Conversely, insufficient or excessive potentials result in a scarcity of active sites or structural collapse, respectively. These findings provide fresh insights into the evolutionary mechanism of sulfide-based catalysts during anodic reactions and offer an effective strategy for constructing high-performance HMFOR electrocatalytic systems via potential-regulated reconstruction.
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DOI
高影响因子
RARE METALS
·
2025
·
IF 11
Huang Huoshuai,Wei Zhidong,Yan Jiawei,Chi Jiasheng,Su Qianxiang,Ma Linlin,Chen Mingxia,Jiang Zhi,Sun Yangzhou,Shangguan Wenfeng
Photocatalytic hydrogen evolution, a promising clean energy conversion technology, faces efficiency limitations due to the mismatched timescales between sub-picosecond bulk photocarrier recombination and microsecond-scale surface reaction. Herein, a dual-strategy involving selenium decoration and NiS x cocatalyst loading was proposed to ameliorate the carrier dynamics bottleneck in CdS-based photocatalysts. The in situ loading of NiS x cocatalysts established an interfacial built-in electric field (BIEF) that enabled spatially oriented carrier separation and transfer, while the selenium modification optimized the light absorption range and Fermi energy level, obtaining an increase in the photocarrier concentration and further modulated the BIEF. Femtosecond transient absorption spectroscopy revealed a dual-channel carrier dynamics enhancement mechanism that BIEF-driven directional charge migration synergistically coupled with NiS x -mediated holes trapping. This synergistic effect achieved an approximately tenfold enhancement of hydrogen evolution rate (461.71 μmol h −1 ) relative to that of bare CdS under visible light (> 420 nm). This study elucidated the regulatory mechanism of element decoration and cocatalyst loading on carrier dynamics, providing an insight for designing high-performance photocatalysts.
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
Zhiqiang Zhang,Xiaofeng Lin,Shuli Tang,Qitong Huang
The development of highly active and stable electrocatalysts is essential to solve energy and environmental problems and realize sustainable social and economic development. Herein, we synthesized a bimetallic sulfide material by a kinetically controlled low-temperature solid-phase reaction. The bimetallic sulfide improves the conductivity of the electrocatalysts by optimized electronic structure, and the coupling effect at the heterogeneous interface of WS 2 and NiS x increases the charge density on the S site at W– S –Ni, making it easier for the electrocatalysts to trap the active material in solution. In addition, nanosheet clusters expose abundant catalytic sites, which together improve hydrogen evolution reaction (HER) for catalytic activity . Optimized WS 2 /NiS x composite show near-precious metal catalyst activity with an overpotential at 10 mA cm −2 of only 72 mV in alkaline media , which exhibits excellent catalytic stability and outperforms most non-precious metal electrocatalysts.
研究领域:
材料科学
·
能源化学
✓ 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）