CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Fei Wang,Wenbin Li,Zengtao Lv,Linxing Meng,Baiyang Zhou,Ting Ding,Zhuo Zhang,Zaixing Yang
Although the built-in local electric field (LEF) triggered by surface oxygen vacancy (O V ) plays a positive role in photoelectrochemical (PEC) water splitting, the migration of electrons is inevitably retarded and trapped by internal O V . In this work, Se/Cu co-doped BiOCl nanosheets (NSs) were synthesized for PEC seawater reduction. The results reveal that, firstly, the O V of BiOCl NSs could be completely eliminated and filled by Se atoms. Secondly, the lattice of BiOCl is distorted by Se/Cu atoms, resulting in an atomic-scale anisotropic LEF that varies in intensity about twice around the Se/Cu atoms, and a synergistic catalytic optimization for H 2 evolution. Thirdly, the gap width of BiOCl is not narrowed after Cu/Se-doping, but the defect levels appear inside the band gap, thus the photoelectrons maintain high kinetics even when excited by visible light. Moreover, the center of Cu 3 d mid-gap state of the Cu/Se co-doped sample has an upward shift than that of the only Cu-doped one. Resultantly, Cu 1% Se 1% BiOCl NSs demonstrate a highly enhanced PEC current density of −0.015 mA/cm 2 at −0.2 V RHE in natural seawater under AM 1.5G solar illumination. This work provides a practical strategy towards non-O V induced anisotropic LEF, and a durable PEC cathode for seawater reduction.
研究领域:
材料科学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Sheng Liao,Shunli Shi,Jie Hu,Yunpeng Zeng,Weiming Xiao,Shuhua Wang,Chao Chen
Hydrogen production through water electrolysis is a crucial method for generating hydrogen; however, the oxygen evolution reaction (OER) requires high reaction potentials, leading to significant electrical energy consumption. In contrast, aldehyde oxidation at ultra-low potentials offers a promising alternative to OER. Coupling aldehyde oxidation with the hydrogen evolution reaction (HER) forms an ideal system for hydrogen production, simultaneously generating high value-added oxidation products and avoiding less economically valuable O 2 . This study employs a photoelectrocatalytic system to drive the oxidation of formalin solutions in a safe and sustainable manner. Utilizing water as the oxidant, the system provides a viable strategy for dual hydrogen production and organic synthesis in neutral media. Under an applied bias voltage of 0.6 V vs. Ag/AgCl and simulated sunlight of 100 mW cm −2 , the BiVO 4 photoanode achieved 83% selectivity for formic acid production. Furthermore, dual hydrogen production was realized at both the anode and cathode, with an apparent Faradaic efficiency of 35%. This work presents an energy-saving and environmentally friendly pathway for solar hydrogen storage and the production of high value-added chemicals, underscoring the potential application of the photoelectrochemical (PEC) method in coupled systems.
研究领域:
能源科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
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2020
·Vol. 7
·期 14
·2669-2675
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IF 5.958
Shunhang Wei,Xiaoxiang Xu
Nitrogen doping was applied to layered compound LaZrTa3O11 (a wide bandgap semiconductor photocatalyst). Bandgap reductions >2.2 eV were achieved by this modification, which effectively red-shifted the light-absorption edge of LaZrTa3O11 from 300 nm to ∼650 nm. Nitrogen-doped LaZrTa3O11 (i.e., LaZrTa3O11−xNy) was now active for both water-reduction and -oxidation reactions under visible-light illumination (λ ≥400 nm) with good durability and stability. An apparent quantum efficiency (AQE) as high as 0.53% at 420 ± 20 nm was achieved for water-oxidation reactions. Further analyses suggested that its visible-light activity originated mainly from an uplift of the valence band edge as a result of nitrogen incorporation. This strategy to achieve visible-light activity was very inspiring and could be applicable to other layered compounds that are active only under ultraviolet-light illumination.
研究领域:
材料科学
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光化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jiejie Bai,Yue Shi,Aixin Ma,Feifei Liu,Yanru Liu,Caixia Li,Jianping Lai,Lei Wang
The production of three separated, high-value chemicals (H 2 O 2 , urea and H 2 ) from CO 2 , N 2 , and H 2 O represents a significant challenge. It is a prospective and innovative way to simultaneously produce these chemicals in an anion exchange membrane (AEM) electrolyzer, which couples anodic 2e - water oxidation (2e - WOR) and cathodic CO 2 , N 2 and water reduction reaction (CNWRR), but has not yet been realized. Here, we found that bifunctional Cu x Ti 1-x O 2-y catalysts can be employed in the electrochemical production of H 2 O 2 , urea and H 2 from CO 2 , N 2 and water, and the optimized Cu 0.12 Ti 0.88 O 2-y catalyst exhibits an excellent productivity of 11.8 μmol cm −2 min −1 , 0.3 mg cm -2 h −1 and 0.82 mmol cm -2 h −1 for H 2 O 2 , urea and H 2 at 4.0 V (50 mA cm −2 ) in AEM electrolyzer, respectively. Theoretical calculations reveal that the superior performance of the 2e - WOR and CNWRR is attributed to the Cu doping effect, which not only promotes the coupling of *OH but also optimizes the adsorption energy barriers of COOH* and NNH*. It is worth noting that the AEM electrolyzer assembled by bifunctional Cu 0.12 Ti 0.88 O 2-y reaches a current density of 50 mA cm −2 with a cell voltage of 4.0 V and exhibits excellent stability of 50-hour continuous operation.
研究领域:
电化学
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催化
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材料科学
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2020
·
IF 4.473
Yuanxing Wang,Cailing Niu,Yachuan Zhu,Da He,Weixin Huang
Producing syngas from electrochemical reduction of CO2 by renewable energy offers an opportunity to reduce CO2 emissions and provide chemicals and fuels. Herein, we report the careful manipulation of the reduction treatment to synthesize copper nanowire arrays (Cu NAs). By thermal oxidation, copper oxide nanowires were grown on a Cu mesh. Then, thermal reduction and electrochemical reduction were used to reduce copper oxide to Cu with the morphologic features largely preserved. The derived Cu NAs are cost-effective electrocatalysts capable of reducing CO2 and H2O for tunable syngas production. It is demonstrated that syngas, the mixture of H2 and CO, could be attained with a wide range of compositions (from 1:2 to 3:1) from CO2 reduction and H2O reduction on these Cu NAs in aqueous solutions. In addition, Cu NAs show a high current density, 4 mA/cm2, at a low potential, −0.5 V, with a high syngas faradaic efficiency of over 70%. This approach explores a new method that sheds light on tuning the syngas composition from the electrochemical CO2 reduction by Cu-based catalysts.
研究领域:
电化学
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材料科学
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可再生能源
·
催化
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 33
·19531-19538
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IF 10.733
Qi Hu,Guomin Li,Xiaowan Huang,Ziyu Wang,Hengpan Yang,Qianling Zhang,Jianhong Liu,Chuanxin He
Regulation of the electronic structures of metal centers represents a robust strategy for enhancing the activity of electrocatalysts. Herein, we report the crafting of hybrid electrocatalysts comprising both single atomic Ru (SA-Ru) and Ru nanoparticles (NPs) supported on porous N-doped carbon (PC), in which the electronic structures of SA-Ru were effectively optimized by nearby Ru NPs to achieve great enhancement of the hydrogen evolution reaction (HER). The resulting SA-Ru/Ru NPs/PC displayed ultrahigh activity for HER in 1 M KOH with a mass activity of 4.2 mA μgRu−1 at −0.07 V vs. RHE; this activity was 14 times that of commercial Pt/C, representing the largest reported value among the Pt-free electrocatalysts. In addition to the ultrahigh activity, the composite possessed the outstanding stability of 24 h and rapid HER kinetics (i.e. Tafel slope: 31.8 mV dec−1). The experimental and theoretical results matched well with each other and unambiguously indicated that the control over the electronic structures of SA-Ru and the advantageous PC support (i.e. its hierarchical porous nanostructures and superhydrophilic surface) jointly contributed to the exceptional performance.
研究领域:
材料科学
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电化学
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催化
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Li Tongtong,Wang Boran,Cao Yu,Liu Zhexuan,Wang Shaogang,Zhang Qi,Sun Jie,Zhou Guangmin
Hydrogen production by seawater electrolysis is significantly hindered by high energy costs and undesirable detrimental chlorine chemistry in seawater. In this work, energy-saving hydrogen production is reported by chlorine-free seawater splitting coupling tip-enhanced electric field promoted electrocatalytic sulfion oxidation reaction. We present a bifunctional needle-like Co 3 S 4 catalyst grown on nickel foam with a unique tip structure that enhances the kinetic rate by improving the current density in the tip region. The assembled hybrid seawater electrolyzer combines thermodynamically favorable sulfion oxidation and cathodic seawater reduction can enable sustainable hydrogen production at a current density of 100 mA cm −2 for up to 504 h. The hybrid seawater electrolyzer has the potential for scale-up industrial implementation of hydrogen production by seawater electrolysis, which is promising to achieve high economic efficiency and environmental remediation.
研究领域:
化学工程
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材料科学
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电化学
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可再生能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Muhammad Humayun,Habib Ullah,Zhuo-Er Cheng,Asif Ali Tahir,Wei Luo,Chundong Wang
Highly efficient photocatalytic water reduction to evolve hydrogen can be achieved by the construction of Z-scheme systems that mimics natural photosynthesis. However, coupling appropriate semiconductors with suitable water reduction potential still remains challenging. Herein, we report a novel Z-scheme system, based on the Au decorated 5,10,15,20-tetrakis(4-trimethylammoniophenyl) porphyrin tetra(p-toluene sulfonate) functionalized iron-doped carbon nitride . We prepared carbon nitride by varying the amount of iron dopant and then functionalized with porphyrin to obtain heterostructure photocatalyst. Owing to the strong interfacial contact and proper band alignment, a Z-scheme system is fabricated. Finally, we deposited Au nanoparticles over the surface of the as-fabricated Z-scheme system to promote the surface redox properties via efficient charge carrier’s separation and transfer. The 3Au-3 P/30Fe-CN photocatalyst achieved excellent H 2 evolution activity by producing 3172.20 µmol h −1 g −1 under UV–visible irradiation. The calculated quantum efficiencies for 3Au-3 P/30Fe-CN photocatalyst at 365 and 420 nm irradiation wavelengths are 7.2% and 3.26%, respectively. The experimentally observed efficiency of our photocatalyst is supported by the density functional theory simulations in terms of the lowest work function and strong electrostatic interaction among the constituents of Z-scheme system.
研究领域:
材料科学
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光催化
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纳米技术
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物理化学
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2020
·Vol. 11
·期 1
·1-13
·
IF 12.121
Zhao Fulai,Feng Yiyu,Wang Yu,Zhang Xin,Liang Xuejing,Li Zhen,Zhang Fei,Wang Tuo,Gong Jinlong,Feng Wei
The discovery of graphene and graphene-like two-dimensional materials has brought fresh vitality to the field of photocatalysis. Bandgap engineering has always been an effective way to make semiconductors more suitable for specific applications such as photocatalysis and optoelectronics. Achieving control over the bandgap helps to improve the light absorption capacity of the semiconductor materials, thereby improving the photocatalytic performance. This work reports two-dimensional −H/−OH terminal-substituted siligenes (gersiloxenes) with tunable bandgap. All gersiloxenes are direct-gap semiconductors and have wide range of light absorption and suitable band positions for light driven water reduction into H 2 , and CO 2 reduction to CO under mild conditions. The gersiloxene with the best performance can provide a maximum CO production of 6.91 mmol g −1 h −1 , and a high apparent quantum efficiency (AQE) of 5.95% at 420 nm. This work may open up new insights into the discovery, research and application of new two-dimensional materials in photocatalysis.
研究领域:
材料科学
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光催化
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半导体物理
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能源材料
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Pengfei Cheng,Yuanwu Liu,Mario Ziegler,Malte Klingenhof,Dong Wang,Zhang Zhang,Peter Strasser,Peter Schaaf
Photoelectrochemical (PEC) water splitting for H2 production is a possible alternative for fossil energy in the future. However, there exists three problems in PEC water splitting with the silicon (Si) photocathode: poor light absorption of the untreated Si substrate, bad stability in strong acid solution, and poor photocatalytic activity of Si. Here, a strategy of dual interface engineering and photocatalyst deposition is proposed to improve the PEC performance, which consists of fabricating black Si (b-Si) by reactive ion etching, depositing of TiO2 on the b-Si by atomic layer deposition, and growing ReS2 on top of the TiO2 by chemical vapor deposition. Owing to the suitable band alignment of b-Si, TiO2, and ReS2, the ReS2/TiO2/b-Si shows obviously enhanced PEC performance compared to b-Si, TiO2/b-Si, and ReS2/b-Si photocathodes. Results of electrochemical impedance spectroscopy and Mott–Schottky plot analysis demonstrate that the TiO2 layer plays an important role and the charge-transfer kinetics of the system is clearly improved. Transient photocurrent measurements indicate that the ReS2/TiO2/b-Si photocathode has the most remarkable photocurrent response. In addition, the ReS2/TiO2/b-Si photocathode also shows excellent stability after being operated for 25 h.
研究领域:
材料科学
·
电化学
·
可再生能源
·
催化
·
纳米技术
✓ 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）