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FUEL PROCESSING TECHNOLOGY · 2021 · IF 7.033

Highly efficient H2 and S production from H2S decomposition via microwave catalysis over a family of TiO2 modified MoxC microwave catalysts

Jianan Chen,Jun Zhu,Wentao Xu,Yi Chen,Jicheng Zhou

Highly efficient H 2 and S production from copious waste H 2 S is beneficial from both environmental and energy. Whereas, the highly effective direct decomposition of H 2 S reaction faces a gigantic obstacle, that is, there is the severe thermal equilibrium limitation. Herein, a family of TiO 2 modified Mo x C as novel microwave catalysts have been developed. This work demonstrates that Mo 2 C, Mo 2 C-TiO 2 and MoC@TiO 2 microwave catalysts display excellent catalytic performance to recover both valuable H 2 and elemental S from the direct decomposition of H 2 S under microwave irradiation . The optimal H 2 S conversion of MoC@TiO 2 can be as high as 99.9% (almost complete conversion) at 700 °C, which greatly outpaces the corresponding H 2 S equilibrium conversion under microwave irradiation . This result of the chemical equilibrium limitation being broken shows an interesting phenomenon, namely a significant microwave selective catalytic effect by microwave catalysis in H 2 S decomposition reaction . In addition, the apparent activation energy of the Mo 2 C, Mo 2 C-TiO 2 and MoC@TiO 2 microwave catalysts reduced to 18.2 kJ/mol, 16.8 kJ/mol and 15.6 kJ/mol under microwave irradiation. The work supplies a strategy for highly effective valuable H 2 and S production from H 2 S decomposition reaction , and paves a path to high-value utilization of hazardous waste H 2 S resources with energy-saving heating method.

研究领域: 化学工程 · 环境科学 · 能源科学
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Journal of Cleaner Production · 2022 · IF 11.072

An approach on chromium discharge reduction: Effect and mechanism of ketone carboxylic acid as high exhaustion chrome tanning agent

Mai Ouyang,Kehui Hu,Qianwen Jiang,Qingda Yao,Hualong Zhou,Yupei Deng,Yiyue Shen,Fahui Li,Linghua Zhuang,Guowei Wang

Chrome tanning agent is the most widely used tanning agent with the best performances of finished leather , but the traditional chrome tanning process poses severe challenges because of the serious chromium pollution, thus the upgrading of cleaner chrome tanning process is imminent. In order to reduce the residual chromium in wastewater and increase the utilization rate of chrome tanning agent, 4-acetyl-heptanediate (AHA), a high exhaustion chrome auxiliary , was developed and applied in chrome retanning process. The results showed that AHA chrome retanning processes (AHA-6 and AHA-4) significantly reduced the chromium content in wastewater by 48.14% and 47.57%, and increased the chromium content in leather by 102.14% and 82.43%. COD and TDS values decreased by 43.82% and 31.46% with AHA-4 method. The addition of AHA obviously reduced the chromium concentration of wastewater, improved the chromium absorption rate, and promoted the cleaner chrome retanning process, which satisfied with the overall requirements of modern sustainable leather industry. The formation of AHA and chromium (III) was discussed using Gaussian 16 program to explain the high exhaustion chrome tanning agent mechanism. The work will guide on design and preparation of new high exhaustion chromium tanning agents for clean leather production.

研究领域: 化学工程 · 环境科学 · 材料科学
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Advanced Composites and Hybrid Materials · 2023 ·Vol. 6 ·期 5 ·1-13 · IF 20.1

Ferrum-doped nickel selenide @tri-nickel diselenide heterostructure electrocatalysts with efficient and stable water splitting for hydrogen and oxygen production

Luo ZhongKe,Tong LongZhi,Lin Zhiping,Amin R. S.,Ren Junna,El-Khatib K. M.,Wang Chao

To meet the increasing demand for clean energy, environmentally friendly and efficient transition metal selenides (TMSes) electrocatalysts for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) are being developed. There is an urgent need for a rational design of bifunctional non-precious metal catalysts with advanced structure and superior composition. In water splitting for the production of clean hydrogen energy, transition metal selenides have promising applications. We prepare a catalyst by a two-step hydrothermal method, and the crystal structure of the catalysts can be easily adjusted by adjusting the concentration of the selenizing agent; when the concentration of the selenizing agent (Na 2 SeO 3 ) is 0.6 mmol, a phase transition occurred, forming the NiSe@Ni 3 Se 2 heterostructure, reaching a current density of 10 mA cm −2 at an overpotential of 214 mV with a low Tafel slope of 41 mV dec −1 . When the concentration of selenide is increased to 0.6 mmol, the prepared NiFeSe 0.6 -MOF (metal organic framework) demonstrates excellent HER performance. At 10 mA cm −2 current density, the overpotential is only 156 mV. Moreover, the monolithic hydrolysis electrolyzer assemble with NiFeSe 0.6 -MOF as the anode and cathode electrodes shows a low cell voltage of 1.7 V at a current density of 10 mA cm −2 , and almost no attenuation is observed after a 72-h stability test. The excellent electrocatalytic performance of the prepared catalysts is attributed to the formation of nickel selenide heterostructures and the synergistic effect of two-dimensional ferrum-doped MOF, which provide abundant active sites. This study provides a good idea for the development of high activity and high stability catalysts. Graphical Abstract

研究领域: 材料科学 · 电化学 · 能源科学
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Advanced Science · 2023 ·Vol. 10 ·期 26 ·2301872 · IF 15.1

Cable-Car Electrocatalysis to Drive Fully Decoupled Water Splitting

Yuanzheng Long,Cheng Yang,Yulong Wu,Bohan Deng,Ziwei Li,Naveed Hussain,Kuangyu Wang,Ruyue Wang,Xian He,Peng Du,Zeliang Guo,Jialiang Lang,Kai Huang,Hui Wu

The increasing demand for clean energy conversion and storage has increased interest in hydrogen production via electrolytic water splitting. However, the simultaneous production of hydrogen and oxygen in this process poses a challenge in extracting pure hydrogen without using ionic conducting membranes. Researchers have developed various innovative designs to overcome this issue, but continuous water splitting in separated tanks remains a desirable approach. This study presents a novel, continuous roll-to-roll process that enables fully decoupled hydrogen evaluation reaction (HER) and oxygen evolution reaction (OER) in two separate electrolyte tanks. The system utilizes specially designed “cable-car” electrodes (CCE) that cycle between the HER and OER tanks, resulting in continuous hydrogen production with a purity of over 99.9% and Coulombic efficiency of 98% for prolonged periods. This membrane-free water splitting system offers promising prospects for scaled-up industrial-scale green hydrogen production, as it reduces the cost and complexity of the system, and allows for the use of renewable energy sources to power the electrolysis process, thus reducing the carbon footprint of hydrogen production.

CAS / MDL: 12054-48-7
研究领域: 能源科学 · 材料科学 · 环境科学
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Nature Communications · 2025 ·Vol. 16 ·期 1 ·1-12 · IF 15.7

A scalable solar-driven photocatalytic system for separated H2 and O2 production from water

Fu Hui,Wu Yaqiang,Guo Yuhao,Sakurai Takuya,Zhang Qianqian,Liu Yuanyuan,Zheng Zhaoke,Cheng Hefeng,Wang Zeyan,Huang Baibiao,Wang Qian,Domen Kazunari,Wang Peng

Solar-driven photocatalytic water splitting offers a sustainable pathway to produce green hydrogen, yet its practical application encounters several challenges including inefficient photocatalysts, sluggish water oxidation, severe reverse reactions and the necessity of separating produced hydrogen and oxygen gases. Herein, we design and develop a photocatalytic system composed of two separate reaction parts: a hydrogen evolution cell containing halide perovskite photocatalysts (MoSe 2 -loaded CH(NH 2 ) 2 PbBr 3-x I x ) and an oxygen evolution cell containing NiFe-layered double hydroxide modified BiVO 4 photocatalysts. These components are bridged by a I 3 − /I − redox couple to facilitate electron transfer, realizing efficient overall water splitting with a solar-to-hydrogen conversion efficiency of 2.47 ± 0.03%. Additionally, an outdoor scaled-up setup of 692.5 cm 2 achieves an average solar-to-hydrogen conversion efficiency of 1.21% during a week-long test under natural sunlight. By addressing major limitations inherent in conventional photocatalytic systems, such as the cooccurrence of hydrogen and oxygen in a single cell and the resultant severe reverse reactions from hydrogen and oxygen recombination, this work introduces an alternative concept for photocatalytic system design, which enhances both efficiency and practicality.

研究领域: 材料科学 · 能源科学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Integration of ultraviolet irradiation with electrochemical chlorine and hydrogen peroxide production for micropollutant abatement

Yinqiao Zhang,Juhong Zhan,Bin Wang,Jun Huang,Shubo Deng,Gang Yu,Sridhar Komarneni,Yujue Wang

This research evaluated integrating ultraviolet (UV) irradiation with electrochemical chlorine (Cl 2 ) and/or hydrogen peroxide (H 2 O 2 ) production for micropollutant abatement in water treatment. Combining UV with anodic Cl 2 production (E-UV/Cl 2 ) effectively abated gemfibrozil and naproxen, but ineffectively abated ibuprofen due to its low reactivity with chlorine radicals (e.g., ClO• and Cl 2 - •). In comparison, combining UV with cathodic H 2 O 2 production (E-UV/H 2 O 2 ) more effectively abated ibuprofen, but less efficiently abated gemfibrozil and naproxen due to the significant scavenging of •OH by the water matrix. Moreover, simultaneously producing Cl 2 and H 2 O 2 during UV irradiation (E-UV/Cl 2 /H 2 O 2 ) in an undivided reactor did not further enhance micropollutant abatement compared to the E-UV/H 2 O 2 process because of the mutual consumption of anodically generated Cl 2 and cathodic generated H 2 O 2 . In contrast, by separating the anodic and cathodic compartments with an anion exchange membrane and operating the E-UV/Cl 2 /H 2 O 2 process in an anode-to-cathode configuration, all test micropollutants could be adequately abated through the sequential oxidation with the selective chlorine radicals and non-selective •OH in the anodic and cathodic compartments. In general, the concentrations of micropollutants could be abated by 84–100% with a short hydraulic residence time (HRT) of 9.4 min and feasible energy demand (E EO  ≤ 3.15 kWh/m 3 -log) in the selected groundwater and secondary wastewater during the E-UV/Cl 2 /H 2 O 2 process in the divided reactor. The results indicate that different synergistic effects can be obtained for micropollutant abatement by combining UV and electrochemical processes in varying configurations, and the divided E-UV/Cl 2 /H 2 O 2 process is a more robust and energy-efficient method for micropollutant abatement during decentralized water treatment.

研究领域: 环境科学 · 水处理工程
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SCIENCE OF THE TOTAL ENVIRONMENT · 2021 · IF 7.963

Promoting biomethane production from propionate with Fe2O3@carbon nanotubes composites

Zhi-Man Yang,Rong-Bo Guo,Xiao-Huan Dong

Using a batch anaerobic system constructed with 60 mL serum bottles, potential of a composite material with Fe 2 O 3 nanoparticles decorated on carbon nanotubes (CNTs) to enhance biomethane production was investigated. The composites (Fe 2 O 3 @CNTs) with well dispersed Fe 2 O 3 nanoparticles (4.5 nm) were fabricated by a facile thermal decomposition method in a muffle furnace under nitrogen atmosphere. Compared with Fe 2 O 3 , Fe 2 O 3 @CNTs showed a large specific surface area and good electrical conductivity. Supplementation of Fe 2 O 3 @CNTs to the propionate-degrading enrichments enhanced the methane production rate, which was 10.4-fold higher than that in the control experiment without material addition. The addition of Fe 2 O 3 @CNTs also not only showed a clearly electrochemical response to flavin and cytochrome C, but also reduced the electron transfer resistance when compared to the control. Comparative analysis showed that Fe 2 O 3 in Fe 2 O 3 @CNTs played a key role in initiating electrochemical response and triggering rapid methane production, while CNTs functioned as rapid electron conduits to facilitate electron transfer from iron-reducing bacteria (e.g., Acinetobacter , Syntrophomonas , and Geobacter ) to methanogens (e.g. Methanosarcina ).

CAS / MDL: 308068-56-6
研究领域: 环境工程 · 微生物学 · 能源技术
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2021 · IF 19.503

2,5-Bis(hydroxymethyl)furan: A new alternative to HMF for simultaneously electrocatalytic production of FDCA and H2 over CoOOH/Ni electrodes

Bin Zhu,Chunlin Chen,Liyuan Huai,Zhenqiang Zhou,Lei Wang,Jian Zhang

Simultaneous production of value-added 2,5-furandicarboxylic acid (FDCA) and H 2 from the integrated 5-hydroxymethylfurfural (HMF) oxidation and hydrogen evolution reaction by electrocatalysis has drawn tremendous attention due to the significantly improved energy efficiency. However, HMF is not thermally and chemically stable enough to often cause heavy degradation, impeding its storage and industrialization. In this work, a more stable furan molecule, 2,5-bis(hydroxymethyl)furan (BHMF), was employed as the reaction substrate into the coupling system for the first time. By means of facile electrodeposition and subsequent oxidative activation, the standing CoOOH nanosheet electrocatalyst was fabricated to realize a complete BHMF conversion with 90.2 % FDCA yield and 100 % current efficiency for H 2 evolution. The reaction path and apparent activation energies were therefore discussed. Scalable properties and electrochemical durability of CoOOH were evaluated in a continuous flow reactor to harvest gram-level solid FDCA, highlighting the prospect of green coupling electrolysis for industrial application.

研究领域: 化学工程 · 能源科学
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FUEL · 2022 · IF 8.035

High-efficiency hollow Zn0.98Cu0.02Se/ZnS/ZnTiO3 photocatalyst for hydrogen production application

Jiaru Peng,Ying Wang,Jiayu Bai,Dingxuan Ma,Ruiyang Zhao,Jishu Han,Lei Wang

Photocatalytic water splitting utilizes solar energy to produce hydrogen, which is considered as one of the most efficient approaches for solving the current global energy and environmental crises. In this work, hollow ZnTiO 3 nanospheres were prepared by calcination method, then ZnS was loaded onto the surface of ZnTiO 3 . At last, Zn 0.98 Cu 0.02 Se nanocrystals with different concentrations were modified at the outermost layer. The optimal photocatalytic hydrogen evolution amount of Zn 0.98 Cu 0.02 Se/ZnS/ZnTiO 3 reached to 36662.23 μmol·g −1 in 6 h. The construction of ternary photocatalyst effectively improved the utilization rate of light absorption, realized the rapid separation and transfer of electrons, significantly suppressed the recombination of charge carriers and was benificial for the enhancement of photocatalytic hydrogen evolution performance.

研究领域: 材料科学 · 能源科学
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Nano Energy · 2018 · IF 13.12

High efficiency photocatalytic hydrogen production over ternary Cu/TiO2@Ti3C2Tx enabled by low-work-function 2D titanium carbide

Chao Peng,Ping Wei,Xiaoyao Li,Yunpeng Liu,Yonghai Cao,Hongjuan Wang,Hao Yu,Feng Peng,Liyun Zhang,Bingsen Zhang,Kangle Lv

It is of prime importance to harness the transfer and flow of photogenerated electrons and holes to elongate the lifetimes of charge carriers and enhance the activity of semiconductor photocatalyst , which can be achieved by hybridizing the photocatalyst with appropriate cocatalysts with right electronic properties and placement. Herein, MXenes, a young family of two-dimensional transition metal carbides , are exploited as a hole mediator to enhance the photocatalytic activity of TiO 2 . We grow TiO 2 sheets exposing (001) surfaces on layered Ti 3 C 2 T x , and then photodeposited Cu 2 O nanodots on TiO 2 . We experimentally prove that the Ti 3 C 2 T x MXene from the wet HF etching method behaves as a low work function material ( ϕ = 3.4 eV). Thanks to this unique electronic property, the photogenerated electrons on TiO 2 hybridized with Ti 3 C 2 T x accumulate and tunnel to Cu 2 O to reduce it to elemental Cu as a reduction cocatalyst. The resulting Cu/TiO 2 @Ti 3 C 2 T x photocatalyst efficiently split water to produce hydrogen at 860 μmol g −1 h −1 . The results presented here demonstrate the promise of MXene materials in photocatalytic solar energy utilization. The insight into the electronic property of MXene sheds light on the new approach to the rational design of high-efficiency photocatalysts composed of MXenes.

CAS / MDL: 1317-38-0 7664-39-3
研究领域: 材料科学 · 能源化学
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Journal of the American Chemical Society · 2023 · IF 15

Coordination-Promoted Bio-Catechol Electro-Reforming toward Sustainable Polymer Production

Ran Wang,Chong Li,Jianxiang Wu,Wei Du,Tao Jiang,Yizhou Yang,Xuejing Yang,Ming Gong

Sustainable polymer production is essential for a carbon-neutral society. cis,cis-Muconic acid is attracting growing interest as a biomass-derived platform molecule with direct access to adipic acid and terephthalic acid, prominent monomers of commercial polymers. Here, a sustainable route of electro-reforming biorenewable catechol to cis,cis-muconic acid with concurrent H2 production has been proposed. By using a CuO foam electrode, a high cis,cis-muconate yield of 90% and a high faradaic efficiency of 87% can be achieved under ambient conditions without external oxidant. Zn2+ coordination with the catechol is central to the yield and selectivity. In a combinatory analysis via steady-state electrochemical kinetics, in situ spectroscopy, and theoretical calculation, we revealed that the reaction ensemble of catechol electrooxidation involves three major processes of polymerization, ring cleavage, and depolymerization, in which Zn2+ coordination is highly effective in delaying polymerization and promoting ring cleavage toward cis,cis-muconate. The catecholate coordinated to the Zn2+ cations reallocated its electron density with partial structural deformation to accelerate the electron transfer and facilitate the OH– nucleophilic attack. A practical two-electrode system was eventually demonstrated to efficiently and stably electro-reform catechol into isolable cis,cis-muconic acid and hydrogen, providing solutions for polymer sustainability via utilizing alternative biomass resources and electrified processes.

研究领域: 化学工程 · 环境科学 · 材料科学
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-11 · IF 14.7

Enhanced continuous atmospheric water harvesting with scalable hygroscopic gel driven by natural sunlight and wind

Yang Xinge,Chen Zhihui,Xiang Chengjie,Shan He,Wang Ruzhu

Sorption-based atmospheric water harvesting (SAWH) has received unprecedented attention as a future water and energy platform. However, the water productivity of SAWH systems is still constrained by the slow sorption kinetics at material and component levels and inefficient condensation. Here, we report a facile method to prepare hygroscopic interconnected porous gel (HIPG) with fast sorption-desorption kinetics, high scalability and stability, and strong adhesion property for highly efficient SAWH. We further design a solar-wind coupling driven SAWH device with collaborative heat and mass enhancement achieving continuous water production. Concentrated sunlight contributes to enhancing the desorption and condensation synergistically, and natural wind is introduced to drive the device operation and improve the sorption kinetics. The device demonstrated record high working performance of 14.9 L water m −2 day −1 and thermal efficiency of 25.7% in indoor experiments and 3.5–8.9 L water m −2 day −1 in outdoor experiments by solar concentration without any other energy consumption. This work provides an up-and-coming pathway to realize highly efficient and sustainable clean water supply for off-grid and arid regions.

CAS / MDL: 7447-41-8
研究领域: 环境科学 · 材料科学 · 可再生能源 · 水资源管理
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