The MoS_(2)-based materials are a vital class of heterogeneous catalysts for the hydrodeoxygenation of lignin and its model compounds to produce value-added chemicals especially because of their unique selectivity to ...The MoS_(2)-based materials are a vital class of heterogeneous catalysts for the hydrodeoxygenation of lignin and its model compounds to produce value-added chemicals especially because of their unique selectivity to aromatics.The rational design of MoS_(2)-based catalyst greatly depends on the comprehensive understanding of its structure-activity relationship.However,an intensive summary and critical analysis are still scarce to date.In this review,we attempt to provide an in-depth understanding of the interplay of structure,catalysis,and stability of MoS_(2)-based catalysts for lignin hydrodeoxygenation.The recognition of intrinsic active sites on MoS_(2) structure was firstly discussed,followed by the illustration of MoS_(2)-catalyzed hydrodeoxygenation structural models.Afterward,based on the studies on the MoS_(2)-catalyzed lignin model compounds hydrodeoxygenation,the current active site modification strategies including structural modification of monometallic MoS_(2) catalysts and collaborative modification were summarized and emphatically discussed,which aims to elucidate the structure-activity relationship at the atomic-level.The deactivation mechanism and stabilization strategies were also illustrated to provide instructive suggestion for the rational design of efficient and stable MoS_(2)-based catalysts.Finally,the real lignin depolymerization over MoS_(2)-based catalysts was summarized to point out the advantages and difficulties.This review attempts to highlight the remaining challenges and provide some perspectives for the future development of MoS_(2)-based catalysts for lignin hydrodeoxygenation.展开更多
Slickwater-based fracturing fluid has recently garnered significant attention as the major fluid for volumetric fracturing;however,lots of challenges and limitations such as low viscosity,poor salt tolerance,and possi...Slickwater-based fracturing fluid has recently garnered significant attention as the major fluid for volumetric fracturing;however,lots of challenges and limitations such as low viscosity,poor salt tolerance,and possible formation damage hinder the application of the conventional simple slickwater-based fracturing fluid.In addition,nanomaterials have proven to be potential solutions or improvements to a number of challenges associated with the slickwater.In this paper,molybdenum disulfide(MoS_(2))nanosheets were chemically synthesized by hydrothermal method and applied to improve the performance of conventional slickwater-based fracturing fluid.Firstly,the microstructure characteristics and crystal type of the MoS_(2)nanosheets were analyzed by SEM,EDS,TEM,XPS,and Raman spectroscopy techniques.Then,a series of evaluation experiments were carried out to compare the performance of MoS_(2)nanosheet-modified slickwater with the conventional slickwater,including rheology,drag reduction,and sand suspension.Finally,the enhanced imbibition capacity and potential mechanism of the nanosheet-modified slickwater were systematically investigated.The results showed that the self-synthesized MoS_(2)nanosheets displayed a distinct ultrathin flake-like morphology and a lateral size in the range of tens of nanometers.In the nano-composites,each MoS_(2)nanosheet plays the role of cross-linking point,so as to make the spatial structure of the entire system more compact.Moreover,nanosheet-modified slickwater demonstrates more excellent properties in rheology,drag reduction,and sand suspension.The nanosheet-modified slickwater has a higher apparent viscosity after shearing 120 min under 90℃ and 170 s^(−1).The maximum drag reduction rate achieved 76.3%at 20℃,and the sand settling time of proppants with different mesh in the nano-composites was prolonged.Spontaneous imbibition experiments showed that the gel-breaking fluid of nanosheet-modified slickwater exhibited excellent capability of oil-detaching,and increase the oil recovery to∼35.43%.By observing and analyzing the interfacial behavior of MoS_(2)nanosheets under stimulated reservoir conditions,it was found that the presence of an interfacial tension gradient and the formation of a climbing film may play an essential role in the spontaneous imbibition mechanism.This work innovatively uses two-dimensional MoS_(2)nanosheets to modify regular slickwater and confirms the feasibility of flake-like nanomaterials to improve the performance of slickwater.The study also reveals the underlying mechanism of enhanced imbibition efficiency of the nano-composites.展开更多
基金supported by the National Natural Science Foundation of China(22178258,21975181)。
文摘The MoS_(2)-based materials are a vital class of heterogeneous catalysts for the hydrodeoxygenation of lignin and its model compounds to produce value-added chemicals especially because of their unique selectivity to aromatics.The rational design of MoS_(2)-based catalyst greatly depends on the comprehensive understanding of its structure-activity relationship.However,an intensive summary and critical analysis are still scarce to date.In this review,we attempt to provide an in-depth understanding of the interplay of structure,catalysis,and stability of MoS_(2)-based catalysts for lignin hydrodeoxygenation.The recognition of intrinsic active sites on MoS_(2) structure was firstly discussed,followed by the illustration of MoS_(2)-catalyzed hydrodeoxygenation structural models.Afterward,based on the studies on the MoS_(2)-catalyzed lignin model compounds hydrodeoxygenation,the current active site modification strategies including structural modification of monometallic MoS_(2) catalysts and collaborative modification were summarized and emphatically discussed,which aims to elucidate the structure-activity relationship at the atomic-level.The deactivation mechanism and stabilization strategies were also illustrated to provide instructive suggestion for the rational design of efficient and stable MoS_(2)-based catalysts.Finally,the real lignin depolymerization over MoS_(2)-based catalysts was summarized to point out the advantages and difficulties.This review attempts to highlight the remaining challenges and provide some perspectives for the future development of MoS_(2)-based catalysts for lignin hydrodeoxygenation.
基金This research was financially supported by the National Natural Science Foundation of China(Grant Nos.52004306 and 52174045)the Strategic Cooperation Technology Projects of CNPC and CUPB(Grant Nos.ZLZX2020-01 and ZLZX2020-02)the National Sciencea and Technology Major Projects of China(Grant Nos.2016ZX05030005and 2016ZX05051003).
文摘Slickwater-based fracturing fluid has recently garnered significant attention as the major fluid for volumetric fracturing;however,lots of challenges and limitations such as low viscosity,poor salt tolerance,and possible formation damage hinder the application of the conventional simple slickwater-based fracturing fluid.In addition,nanomaterials have proven to be potential solutions or improvements to a number of challenges associated with the slickwater.In this paper,molybdenum disulfide(MoS_(2))nanosheets were chemically synthesized by hydrothermal method and applied to improve the performance of conventional slickwater-based fracturing fluid.Firstly,the microstructure characteristics and crystal type of the MoS_(2)nanosheets were analyzed by SEM,EDS,TEM,XPS,and Raman spectroscopy techniques.Then,a series of evaluation experiments were carried out to compare the performance of MoS_(2)nanosheet-modified slickwater with the conventional slickwater,including rheology,drag reduction,and sand suspension.Finally,the enhanced imbibition capacity and potential mechanism of the nanosheet-modified slickwater were systematically investigated.The results showed that the self-synthesized MoS_(2)nanosheets displayed a distinct ultrathin flake-like morphology and a lateral size in the range of tens of nanometers.In the nano-composites,each MoS_(2)nanosheet plays the role of cross-linking point,so as to make the spatial structure of the entire system more compact.Moreover,nanosheet-modified slickwater demonstrates more excellent properties in rheology,drag reduction,and sand suspension.The nanosheet-modified slickwater has a higher apparent viscosity after shearing 120 min under 90℃ and 170 s^(−1).The maximum drag reduction rate achieved 76.3%at 20℃,and the sand settling time of proppants with different mesh in the nano-composites was prolonged.Spontaneous imbibition experiments showed that the gel-breaking fluid of nanosheet-modified slickwater exhibited excellent capability of oil-detaching,and increase the oil recovery to∼35.43%.By observing and analyzing the interfacial behavior of MoS_(2)nanosheets under stimulated reservoir conditions,it was found that the presence of an interfacial tension gradient and the formation of a climbing film may play an essential role in the spontaneous imbibition mechanism.This work innovatively uses two-dimensional MoS_(2)nanosheets to modify regular slickwater and confirms the feasibility of flake-like nanomaterials to improve the performance of slickwater.The study also reveals the underlying mechanism of enhanced imbibition efficiency of the nano-composites.
