ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2021
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IF 9.028
Weiting Yu,He Jiang,Jinhui Fang,Shuang Song
Reducing the Pd loading on electrodes is critical in the electrocatalytic hydrodechlorination (EHDC) of chlorinated organic compounds (COCs). The EHDC reaction of COCs on Pd involves three steps: H* formation, H* adsorption, and dechlorination. It has been established that the initial hydrogen evolution reaction (HER) occurs on Pd0 and the dechlorination steps occur on Pd2+. A strategy is proposed to design new electrodes by adding a reducible HER-active interlayer to replace Pd0, fulfilling the responsibility of producing hydrogen, and to facilitate the formation of more Pd2+ for following C–Cl bond cleavage. Keeping the atomic hydrogen adsorption energy on the Pd/interlayer similar to that on pure Pd is also necessary for H* adsorption as well as to maintain a high EHDC activity. For the first time, the NiCo2O4-interlayer-modified Pd/Ni-foam electrode was applied in the EHDC of COCs, which enhanced the EHDC efficiency to 100% within 90 min and reduced 88.6% of Pd consumption. The Pd/NiCo2O4/Ni-foam electrode with enhanced EHDC activity was also observed with almost 100% product selectivity and good stability. A synergistic mechanism is proposed for the enhanced EHDC activity on the Pd/NiCo2O4/Ni-foam. This work offers a simple and useful strategy to design robust electrocatalysts for the EHDC of COCs.
研究领域:
化学
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环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
Journal of Physical Chemistry C
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2021
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IF 4.126
Lu Zhang,Guojun Yuan,Xinyu Wang,Jianliang Bai,Yaqing Zhu,Lili Ren
Environmental pressure gives potential for the application of transition metal phosphides (TMPs), which serve as efficient degradation catalysts. Although various efforts are advocated to obtain high activity, it is still difficult for phosphides to exhibit cycle performance in hydrodechlorination (HDC), limiting their practical development. By linking the changes in the oxidation state of MoP before and after HDC with its catalytic performance, the Mo–P–O bond is found to be the active catalytic site, not only promoting electron transfer but also forming the defect-rich structure. Based on this, H2O2-treated MoP after HDC reached a performance of 19.9%, and the activity could be restored after multiple cycle reactions, while the untreated one still had poor performance, demonstrating that carrying out the H2O2 treatment process can realize the recycling of MoP, which is of importance for industrial application of catalysts.
研究领域:
化学
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环境科学
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材料科学
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DOI
高影响因子
RSC Advances
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2016
·Vol. 6
·期 9
·7413-7418
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IF 3.289
Xiaomeng Liu,Lili Ren
Molybdenum phosphide (MoP), synthesized by combining with polyethylene glycol (PEG), shows 4 to 5 times superior activity than conventional MoP for hydrodechlorination of trichloroethylene (TCE). We investigated the effect of PEG average molecular mass on the catalytic activity of MoP, and found that when the average molecular mass of PEG was 8000, the MoP catalyst gave the highest activity. Through X-ray diffraction (XRD), N2 adsorption–desorption, transmission electron microscopy (TEM), scanning electron microscopy (SEM), and H2 temperature-program reduction (H2-TPR), the effect of PEG was investigated. The results showed that the addition of PEG changed MoP from the original flat structure to a lamellar structure, and indeed improved the growth of the (101) and (102) crystal planes (the possible crystal planes of high activity) and restrained the (100) and (201) crystal planes (the possible crystal planes of low activity). This leads to the high catalytic performance of MoP modified with PEG.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
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2016
·Vol. 6
·期 110
·109023-109029
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IF 3.289
Lijuan Lan,Fanglin Du,Chuanhai Xia
Carbon nanotubes (CNTs) supported Pd catalysts (1 wt% and 5 wt%) were prepared by a conventional impregnation method and tested in liquid-phase hydrodechlorination (HDC) of para-chlorophenol (p-CP) under mild conditions (313 K and atmospheric pressure) with H2. CNTs as a catalyst support offered better performance than activated carbon (AC). The conversion of p-CP reached 72% and 82% over 5 wt% Pd/AC and 5 wt% Pd/CNTs, respectively, within 30 min. When the content of Pd was reduced to 1 wt%, the conversion of p-CP over Pd/AC and Pd/CNTs was 55% and 83%, respectively. The mechanism of this phenomenon was studied through catalyst characterization (XRD, TEM, and BET). The abovementioned results indicated that the different activities of the catalysts over different supports mainly resulted from the porous structure of the supports and nanoparticle diameters of the active metal.
研究领域:
催化化学
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环境科学
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产品关联
DOI
高影响因子
ACS Applied Nano Materials
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2023
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IF 5.9
Xin Ning,Heming Wang,Ganghua Zhou,Longyun Zhang,Yanju Yang,Jingya Sun,Xiaozhi Wang
Ni catalysts decorated with trace Rh supported on γ-Al2O3 were prepared by the co-impregnation method. To obtain the Ni–Rh nanoparticles with different nanostructures and chemical compositions, bimetallic catalysts with varied Ni/Rh molar ratios were prepared. For comparison, monometallic Ni/γ-Al2O3 and Rh/γ-Al2O3 catalysts were also prepared by the impregnation method. The selective gas phase catalytic hydrodechlorination of 1,2-dichloroethane to ethylene was used to evaluate catalytic performances of the catalysts. The catalysts were characterized by X-ray diffraction, N2 adsorption, X-ray photoelectron spectroscopy, H2 temperature-programmed reduction, transmission electron microscopy–energy-dispersive X-ray, and CO chemisorption. It was found that the introduction of Rh to Ni catalyst facilitated the generation of spillover hydrogen which could enhance the ability of the Ni catalyst for H2 activation. In bimetallic catalysts, there was an intimate interaction between Ni and Rh, and isolated Rh sites were formed due to the dilution effect of Ni. Accordingly, compared with the monometallic Ni catalyst for gas phase catalytic hydrodechlorination of 1,2-dichloroethane, the bimetallic Ni–Rh(800)/γ-Al2O3 catalyst exhibited markedly higher 1,2-dichloroethane conversion (37%) and comparable selectivity to ethylene (95%). The findings in this study indicate that Ni–Rh/γ-Al2O3 with trace Rh can be used as a promising catalyst for highly effective and selective catalytic hydrodechlorination of chlorinated hydrocarbons.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
ChemistrySelect
·
2023
·Vol. 8
·期 48
·e202301171
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IF 2.1
Xinyu Wang,Lu Zhang,Guojun Yuan,Jianliang Bai,Yaqing Zhu,Lili Ren
Graphical The mechanism diagram demonstrates that the hydrodechlorination (HDC) reaction of carbon, oxygen co-doped MoP catalyst for trichloroethylene (TCE) shown as the above. Trichloroethylene (TCE) plays an important role in industrial production. However, humans are now suffering the effects of trichloroethylene being released directly into the environment. Therefore, it is urgent to explore effective methods for the degradation of trichloroethylene. Hydrodechlorination (HDC) reaction is considered a green, beneficial and promising technology due to its high selectivity, environmental tenderness and product recovery. Noble metal catalysts are considered as the benchmark catalysts for catalytic processes, but their wide application is limited by their low abundance and low stability. Phosphide has been paid more and more attention in HDC field because of its excellent catalytic performance. In view of the important role of O in the catalytic process, the preparation of C, O co-doped MoP was realized through the co-modification of EDTA and glucose. In the case of changing the molar ratio of MoP to the surface modifier, MOP−C−O (50 %) can achieve the best catalytic efficiency. Even compared with some reported catalysts, it has a very large catalytic advantage. In summary, the C, O co-doped MoP catalyst proposed in this paper provides guidance for the preparation of the same type of catalyst. The harms caused by organic chlorides to the human body and the environment make the problem of how to degrade organic chlorides particularly urgent. Phosphides have gradually attracted attention in HDC due to their high catalytic performance. In view of the important role of O in catalytic process, the preparation of C, O co-doped MoP was achieved by the synergistic modification of EDTA and glucose. Compared with unmodified MoP, the doping of carbon and oxygen in MoP−C−O ensure that more active sites are exposed on the surface. At the same time, the high dispersion of MoP on the carbon matrix increases the specific surface area of MoP−C−O, which is more conducive to the adsorption of reactants on the surface, thereby effectively improving the catalytic activity of the modified MoP−C−O. In the case of changing the molar ratio of MoP and surface modifier, the best activity of MoP−C−O (50 %) reaches 57.80 %, which is 2.3 times higher than that of MoP catalyst.
研究领域:
环境科学
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催化化学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Junjing Li,Menghua Yin,Yu Wang,Liang Wang
In order to change the mass transfer efficiency of conventional flat plate electrodes in the catalytic process, a new filtered Pd@Ti electrode has been prepared. The results indicated that the filtered Pd@Ti electrode had the best removal efficiency of 99.59% on diclofenac (DCF) at the flux of 40.85 L/m 2 ∙h -1 . Compared to unfiltered Pd@Ti electrodes, the removal efficiency was 1.18 times higher, the current efficiency was 2.15 times higher and the cost of electricity was 69.05% lower. The electrocatalytic hydrodechlorination process of DCF by filtered Pd@Ti electrode mainly relies on indirect reductive dechlorination by H* adsorbed on the electrode surface. The removal efficiency of the filtered Pd@Ti electrode remained above 80% after six cycles. The removal mechanism and reaction pathway of filtered Pd@Ti electrode for dechlorination of different chlorinated PPCPs were proposed. Furthermore, the ecotoxicity of chlorinated PPCPs and their products were evaluated by using the toxicity estimation software tool (T.E.S.T.) model. This study confirmed the promising application of filtered Pd@Ti electrodes for the removal and detoxification of chlorinated PPCPs in wastewater.
研究领域:
环境工程
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水处理
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电化学
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毒理学
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产品关联
DOI
高影响因子
ACS ES&T Engineering
·
2025
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IF 6.7
Hehe Qian,Tinghui Ma,Lili Shi,Shu Yan,Haisong Cui,Xueqing Luo,Fang Chen,Yuetan Su,Zhongbiao Wu,Xiaole Weng
Electrocatalytic hydrodechlorination (EHDC) is a promising strategy for remediating chlorinated organic pollutants by utilizing reactive hydrogen (H*) to cleave C–Cl bonds. Addressing the challenge of simultaneously optimizing H* generation and targeted pollutant adsorption/activation, this work introduces synergistic surface engineering of RuPd alloy nanocatalysts. Compositionally controlled RuPd nanoparticles (RuPd2, Ru2Pd3, and Ru2Pd) were synthesized via seed-mediated growth, yielding uniform sub-3.5 nm nanoparticles with homogeneous elemental distribution. The optimal RuPd2 electrocatalysts achieved 97.1% 2-chlorophenol conversion within 6 h at −0.85 V vs Ag/AgCl, exhibiting a mass activity of 28.3 min–1 g–1Pd, representing a 5.6-fold enhancement over monometallic Pd. Moreover, RuPd2 demonstrated enhanced durability, maintaining performance with less than 5% efficiency loss over 10 cycles. This enhanced EHDC performance originated from dual synergistic effects. Electron transfer from Ru to Pd facilitated H* generation kinetics, evidenced by a near-optimal ΔGH* (−0.25 eV) at Pd–Pd–Pd hollow sites, while Ru-rich surface domains significantly strengthened 2-chlorophenol adsorption and elongated the C–Cl bond to facilitate dechlorination. These spatially separated synergistic sites collectively achieve higher EHDC efficiency, establishing a unified catalyst design strategy that effectively orchestrates coupled surface processes, and provides a significant advance for efficient EHDC technology with broad environmental remediation implications.
研究领域:
环境催化
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纳米材料化学
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污染物降解
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电化学
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表面科学
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能源与环境工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Guoshuai Liu,Shanshan He,Hua Zou,Shijie You
Electrocatalytic hydrodechlorination (EHDC) is a promising approach for decomposing chlorinated organic compounds in water treatment. However, the efficiency of EHDC is constrained by kinetic mismatch between C−Cl bond cleavage and atomic hydrogen (H*) utilization. Herein, we develop a heterostructured Pd-H x WO 3 electrocatalyst with Pd nanoparticles (Pd NPs) anchored on H x WO 3 substrate, which can efficiently decompose 2,4-dichlorophenol (2,4-DCP) by taking advantage of the hydrogen spillover effect. Specifically, the resulting Pd-H x WO 3 electrocatalyst exhibits superior dechlorination rate constant ( k = 1.142 h −1 ) and Faradic efficiency (FE = 10.1 %) than monometallic Pd ( k = 0.3600 h −1 , FE = 3.74 %) and bare H x WO 3 ( k = 0.1167 h −1 , FE = 2.11 %), along with exceptional pH adaptability and stability. Electron spin resonance (ESR) and electrochemical and kinetic isotope effect (KIE) measurements indicate that the transport of the H* from H x WO 3 to Pd NPs is the key to enhanced EHDC performance. Theoretical studies reveal that the Volmer step of water dissociation to produce H* is more favorable due to lower transition state (TS) energy (0.344 eV) on H x WO 3 than that on Pd (TS = 0.532 eV). Furthermore, the interfacial electron redistribution in Pd-H x WO 3 lowers the thermodynamic (Δ G = 0.207 eV) and kinetic (Δ G = 0.239 eV) barriers for H* transfer from the internal site of H x WO 3 to interfacial Pd sites, thereby facilitating the proton-coupled electron transfer (PCET)-mediated EHDC on Pd site. This work provides a new proof-in-concept demonstration for designing hydrogen spillover-integrated electrocatalysts to enhance H* generation-transfer-utilization in EHDC for water decontamination.
研究领域:
环境化学
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电催化
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水净化
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材料科学
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可持续化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）