2024 Vol. 9, No. 1

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From the perspective of experimental practice: High-throughput computational screening in photocatalysis
Yunxuan Zhao, Junyu Gao, Xuanang Bian, Han Tang, Tierui Zhang
2024, 9(1): 1-6. doi: 10.1016/j.gee.2023.05.008
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Photocatalysis, a critical strategy for harvesting sunlight to address energy demand and environmental concerns, is underpinned by the discovery of high-performance photocatalysts, thereby how to design photocatalysts is now generating widespread interest in boosting the conversion efficiency of solar energy. In the past decade, computational technologies and theoretical simulations have led to a major leap in the development of high-throughput computational screening strategies for novel high-efficiency photocatalysts. In this viewpoint, we started with introducing the challenges of photocatalysis from the view of experimental practice, especially the inefficiency of the traditional “trial and error” method. Subsequently, a cross-sectional comparison between experimental and high-throughput computational screening for photocatalysis is presented and discussed in detail. On the basis of the current experimental progress in photocatalysis, we also exemplified the various challenges associated with high-throughput computational screening strategies. Finally, we offered a preferred high-throughput computational screening procedure for photocatalysts from an experimental practice perspective (model construction and screening, standardized experiments, assessment and revision), with the aim of a better correlation of high-throughput simulations and experimental practices, motivating to search for better descriptors.
Review articles
Fullerenes and derivatives as electrocatalysts: Promises and challenges
Kun Guo, Ning Li, Lipiao Bao, Xing Lu
2024, 9(1): 7-27. doi: 10.1016/j.gee.2022.11.002
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Carbon-based metal-free nanomaterials are promising alternatives to precious metals as electrocatalysts of key energy storage and conversion technologies. Of paramount significance are the establishment of design principles by understanding the catalytic mechanisms and identifying the active sites. Distinct from sp2-conjugated graphene and carbon nanotube, fullerene possesses unique characteristics that are growingly being discovered and exploited by the electrocatalysis community. For instance, the well-defined atomic and molecular structures, the good electron affinity to tune the electronic structures of other substances, the intermolecular self-assembly into superlattices, and the on-demand chemical modification have endowed fullerene with incomparable advantages as electrocatalysts that are otherwise not applicable to other carbon materials. As increasing studies are being reported on this intriguing topic, it is necessary to provide a state-of-the-art overview of the recent progress. This review takes such an initiative by summarizing the promises and challenges in the electrocatalytic applications of fullerene and its derivatives. The content is structured according to the composition and structure of fullerene, including intact fullerene (e.g., fullerene composite and superlattices) and fullerene derivatives (e.g., doped, endohedral, and disintegrated fullerene). The synthesis, characterization, catalytic mechanisms, and deficiencies of these fullerene-based materials are explicitly elaborated. We conclude it by sharing our perspectives on the key aspects that future efforts shall consider.
Valorization of Camellia oleifera oil processing byproducts to value-added chemicals and biobased materials: A critical review
Xudong Liu, Yiying Wu, Yang Gao, Zhicheng Jiang, Zicheng Zhao, Wenquan Zeng, Mingyu Xie, Sisi Liu, Rukuan Liu, Yan Chao, Suli Nie, Aihua Zhang, Changzhu Li, Zhihong Xiao
2024, 9(1): 28-53. doi: 10.1016/j.gee.2022.12.002
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The C. oleifera oil processing industry generates large amounts of solid wastes, including C. oleifera shell (COS) and C. oleifera cake (COC). Distinct from generally acknowledged lignocellulosic biomass (corn stover, bamboo, birch, etc.), Camellia wastes contain diverse bioactive substances in addition to the abundant lignocellulosic components, and thus, the biorefinery utilization of C. oleifera processing byproducts involves complicated processing technologies. This review first summarizes various technologies for extracting and converting the main components in C. oleifera oil processing byproducts into value-added chemicals and biobased materials, as well as their potential applications. Microwave, ultrasound, and Soxhlet extractions are compared for the extraction of functional bioactive components (tannin, flavonoid, saponin, etc.), while solvothermal conversion and pyrolysis are discussed for the conversion of lignocellulosic components into value-added chemicals. The application areas of these chemicals according to their properties are introduced in detail, including utilizing antioxidant and anti-inflammatory properties of the bioactive substances for the specific application, as well as drop-in chemicals for the substitution of unrenewable fossil fuel-derived products. In addition to chemical production, biochar fabricated from COS and its applications in the fields of adsorption, supercapacitor, soil remediation and wood composites are comprehensively reviewed and discussed. Finally, based on the compositions and structural characteristics of C. oleifera byproducts, the development of full-component valorization strategies and the expansion of the application fields are proposed.
Machine learning for membrane design and discovery
Haoyu Yin, Muzi Xu, Zhiyao Luo, Xiaotian Bi, Jiali Li, Sui Zhang, Xiaonan Wang
2024, 9(1): 54-70. doi: 10.1016/j.gee.2022.12.001
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Membrane technologies are becoming increasingly versatile and helpful today for sustainable development. Machine Learning (ML), an essential branch of artificial intelligence (AI), has substantially impacted the research and development norm of new materials for energy and environment. This review provides an overview and perspectives on ML methodologies and their applications in membrane design and discovery. A brief overview of membrane technologies is first provided with the current bottlenecks and potential solutions. Through an applications-based perspective of AI-aided membrane design and discovery, we further show how ML strategies are applied to the membrane discovery cycle (including membrane material design, membrane application, membrane process design, and knowledge extraction), in various membrane systems, ranging from gas, liquid, and fuel cell separation membranes. Furthermore, the best practices of integrating ML methods and specific application targets in membrane design and discovery are presented with an ideal paradigm proposed. The challenges to be addressed and prospects of AI applications in membrane discovery are also highlighted in the end.
Research papers
Thin polymer electrolyte with MXene functional layer for uniform Li+ deposition in all-solid-state lithium battery
Weijie Kou, Yafang Zhang, Wenjia Wu, Zibiao Guo, Quanxian Hua, Jingtao Wang
2024, 9(1): 71-80. doi: 10.1016/j.gee.2022.05.002
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Solid polymer electrolyte (SPE) shows great potential for all-solid-state batteries because of the inherent safety and flexibility; however, the unfavourable Li+ deposition and large thickness hamper its development and application. Herein, a laminar MXene functional layer‒thin SPE layer‒cathode integration (MXene-PEO-LFP) is designed and fabricated. The MXene functional layer formed by stacking rigid MXene nanosheets imparts higher compressive strength relative to PEO electrolyte layer. And the abundant negatively-charged groups on MXene functional layer effectively repel anions and attract cations to adjust the charge distribution behavior at electrolyte–anode interface. Furthermore, the functional layer with rich lithiophilic groups and outstanding electronic conductivity results in low Li nucleation overpotential and nucleation energy barrier. In consequence, the cell assembled with MXene-PEO-LFP, where the PEO electrolyte layer is only 12 μm, much thinner than most solid electrolytes, exhibits uniform, dendrite-free Li+ deposition and excellent cycling stability. High capacity (142.8 mAh g-1), stable operation of 140 cycles (capacity decay per cycle, 0.065%), and low polarization potential (0.5 C) are obtained in this Li|MXene-PEO-LFP cell, which is superior to most PEO-based electrolytes under identical condition. This integrated design may provide a strategy for the large-scale application of thin polymer electrolytes in all-solid-state battery.
Electro-spraying/spinning: A novel battery manufacturing technology
Zhuan Hu, Jiaxin Hao, Dongyang Shen, Caitian Gao, Zhaomeng Liu, Jianguo Zhao, Bingan Lu
2024, 9(1): 81-88. doi: 10.1016/j.gee.2022.05.004
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Lithium-ion battery (LIB) industry seems to have met its bottle neck in cutting down producing costs even though much efforts have been put into building a complete industrial chain. Actually, manufacturing methods can greatly affect the cost of battery production. Up to now, lithium ion battery producers still adopt manufacturing methods with cumbersome sub-components preparing processes and costly assembling procedures, which will undoubtedly elevate the producing cost. Herein, we propose a novel approach to directly assemble battery components (cathode, anode and separator) in an integrated way using electro-spraying and electro-spinning technologies. More importantly, this novel battery manufacturing method can produce LIBs in large scale, and the products show excellent mechanical strength, flexibility, thermal stability and electrolyte wettability. Additionally, the performance of the as-prepaed LiFePO4||graphite full cell produced by this new method is comparable or even better than that produced by conventional manufacturing approach. In brief, this work provides a new promising technology to prepare LIBs with low cost and better performance.
Superwetting Ag/α-Fe2O3 anchored mesh with enhanced photocatalytic and antibacterial activities for efficient water purification
Jiakai Li, Changpeng Lv, Jiajia Song, Xiaoling Zhang, Xizhen Huang, Yingzhuo Ma, Haijie Cao, Na Liu
2024, 9(1): 89-103. doi: 10.1016/j.gee.2022.05.005
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Superwetting materials have drawn unprecedented attention in the treatment of oily wastewater due to their preferable anti-fouling property and selective oil/water separation. However, it is still a challenge to fabricate multifunctional and environmentally friendly materials, which can be stably applied to purify the actual complicated wastewater. Here, a Ag/α-Fe2O3 heterostructure anchored copper mesh was intentionally synthesized using a facile two-step hydrothermal method. The resultant mesh with superhydrophilicity and underwater superoleophobicity was capable of separating various oil/water mixtures with superior separation efficiency and high permeation flux driven by gravity. Benefiting from the joint effects of the smaller band gap of Ag/α-Fe2O3 heterojunction, inherent antibacterial capacity of α-Fe2O3 and Ag nanoparticles, favorable conductive substrate, as well as the hierarchical structure with superwettability, such mesh presented remarkably enhanced degradation capability toward organic dyes under visible light irradiation and antibacterial activity against both Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus) compared with the pure α-Fe2O3 coated mesh. Impressively, the mesh exhibited bifunctional water purification performance, in which organic dyes were eliminated simultaneously from water during oil/water separation in one filtration process. More importantly, this mesh behaved exceptional chemical resistance, mechanical stability and long-term reusability. Therefore, this material with multifunctional integration may hold promising potential for steady water purification in practice.
Linear paired electrolysis of furfural to furoic acid at both anode and cathode in a multiple redox mediated system
Xinxin Li, Linchuan Cong, Haibo Lin, Fangbing Liu, Xiangxue Fu, Hai-Chao Xu, Nan Lin
2024, 9(1): 104-113. doi: 10.1016/j.gee.2022.05.009
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Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the future. Here, we report a multiple redox-mediated linear paired electrolysis system, combining the hydrogen peroxide mediated cathode process with the I2 mediated anode process, and realize the conversion of furfural to furoic acid in both side of the divided flow cell simultaneously. By reasonably controlling the cathode potential, the undesired water splitting reaction and furfural reduction side reactions are avoided. Under the galvanostatic electrolysis, the two-mediated electrode processes have good compatibility, which reduce the energy consumption by about 22% while improving the electronic efficiency by about 125%. This system provides a green electrochemical synthesis route with commercial prospects.
Role of methoxy and Cα-based substituents in electrochemical oxidation mechanisms and bond cleavage selectivity of β-O-4 lignin model compounds
Yang Zhou, Qiang Zeng, Hongyan He, Kejia Wu, Fuqiao Liu, Xuehui Li
2024, 9(1): 114-125. doi: 10.1016/j.gee.2022.05.006
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In order to better understand the specific substituent effects on the electrochemical oxidation process of β-O-4 bond, a series of methoxyphenyl type β-O-4 dimer model compounds with different localized methoxyl groups, including 2-(2-methoxyphenoxy)-1-phenylethanone, 2-(2-methoxyphenoxy)-1-phenylethanol, 2-(2-methoxyphenoxy)-1-(4-methoxyphenyl)ethanone, 2-(2-methoxyphenoxy)-1-(4-methoxyphenyl)ethanol, 2-(2,6-dimethoxyphenoxy)-1-(4-methoxyphenyl)ethanone, 2-(2,6-dimethoxyphenoxy)-1-(4-methoxyphenyl)ethanol have been selected and their electrochemical properties have been studied experimentally by cyclic voltammetry, and FT-IR spectroelectrochemistry. Combining with electrolysis products distribution analysis and density functional theory calculations, oxidation mechanisms of all six model dimers have been explored. In particular, a total effect from substituents of both para-methoxy (on the aryl ring closing to C) and C-OH on the oxidation mechanisms has been clearly observed, showing a significant selectivity on the C-C bond cleavage induced by electrochemical oxidations.
In-situ construction of abundant active centers on hierarchically porous carbon electrode toward high-performance phosphate electrosorption: Synergistic effect of electric field and capture sites
Peng Zhang, Fukuan Li, Mingming He, Silu Huo, Xueli Zhang, Benqiang Cen, Dezhi Fang, Kexun Li, Hao Wang
2024, 9(1): 126-137. doi: 10.1016/j.gee.2022.06.004
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Phosphate removal is crucial for eutrophication control and water quality improvement. Electro-assisted adsorption, an eco-friendly electrosorption process, exhibited a promising potential for wastewater treatment. However, there are few works focused on phosphate electrosorption, and reported electrodes cannot attach satisfactory removal capacities and rates. Herein, electro-assisted adsorption of phosphate via in-situ construction of La active centers on hierarchically porous carbon (LaPC) has been originally demonstrated. The resulted LaPC composite not only possessed a hierarchically porous structure with uniformly dispersed La active sites, but also provided good conductivity for interfacial electron transfer. The LaPC electrode achieved an ultrahigh phosphate electrosorption capability of 462.01 mg g-1 at 1 V, outperforming most existing electrodes. The superior phosphate removal performance originates from abundant active centers formed by the coupling of electric field and capture sites. Besides, the stability and selectivity toward phosphate capture were maintained well even under comprehensive conditions. Moreover, a series of kinetics and isotherms models were employed to validate the electrosorption process. This work demonstrates a deep understanding and promotes a new level of phosphate electrosorption.
Suppress oxygen evolution of lithium-rich manganese-based cathode materials via an integrated strategy
Wenhua Yu, Yanyan Wang, Aimin Wu, Aikui Li, Zhiwen Qiu, Xufeng Dong, Chuang Dong, Hao Huang
2024, 9(1): 138-151. doi: 10.1016/j.gee.2022.06.001
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Improving the reversibility of anionic redox and inhibiting irreversible oxygen evolution are the main challenges in the application of high reversible capacity Li-rich Mn-based cathode materials. A facile synchronous lithiation strategy combining the advantages of yttrium doping and LiYO2 surface coating is proposed. Yttrium doping effectively suppresses the oxygen evolution during the delithiation process by increasing the energy barrier of oxygen evolution reaction through strong Y–O bond energy. LiYO2 nanocoating has the function of structural constraint and protection, that protecting the lattice oxygen exposed to the surface, thus avoiding irreversible oxidation. As an Li+ conductor, LiYO2 nanocoating can provide a fast Li+ transfer channel, which enables the sample to have excellent rate performance. The synergistic effect of Y doping and nano-LiYO2 coating integration suppresses the oxygen release from the surface, accelerates the diffusion of Li+ from electrolyte to electrode and decreases the interfacial side reactions, enabling the lithium ion batteries to obtain good electrochemical performance. The lithium-ion full cell employing the Y-1 sample (cathode) and commercial graphite (anode) exhibit an excellent specific energy density of 442.9 Wh kg-1 at a current density of 0.1C, with very stable safety performance, which can be used in a wide temperature range (60 to -15 °C) stable operation. This result illustrates a new integration strategy for advanced cathode materials to achieve high specific energy density.
A general synthetic strategy for N, P co-doped graphene supported metal-rich noble metal phosphides for hydrogen generation
Jingwen Ma, Xiang Li, Guangyu Lei, Jun Wang, Juan Wang, Jian Liu, Ming Ke, Yang Li, Chunwen Sun
2024, 9(1): 152-162. doi: 10.1016/j.gee.2022.04.009
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The exploitation of electrocatalysts with high activity and durability for HER is desirable for future energy systems, but it is still a challenge. NMPs have attracted increasing attentions, but the preparation process often needs toxic regents or dangerous reaction conditions. Herein, we develop a general green method to fabricate metal-rich NMPs anchored on NPG through pyrolyzing DNA cross-linked complexes. The obtained Ru2P-NPG exhibits an ultrasmall overpotential of 7 mV at 10 mA cm-2 and ultralow Tafel slope of 33 mV dec-1 in 1.0 mol L-1 KOH, even better than that of commercial Pt/C. In addition, Ru2P-NPG also shows low overpotentials of 29 and 78 mV in 0.5 mol L-1 H2SO4 and 1.0 mol L-1 PBS, respectively. The superior activity can be attributed to the ultrafine dispersion of Ru2P nanoparticles for more accessible sites, more defects formed for abundant active sites, the two-dimensional plane structure for accelerated electron transfer and mass transport, as well as the regulation of electron distribution of the catalyst. Moreover, the synthetic method can also be applied to prepare other metal-rich noble metal phosphides (Pd3P-NPG and Rh2P-NPG), which also exhibits high activity for HER. This work provides an effective strategy for designing NMP-based electrocatalysts.

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